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[Katsuhiko Ariga](https://orcid.org/0000-0002-2445-2955), Wenyan Lyu, Jingwen Song

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[Nanoarchitectonics of molecular machines, biomolecular machines, and microrobots in their collective behaviour](https://mdr.nims.go.jp/datasets/53e85db3-b228-4c22-b218-e05ac78ad1e0)

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Nanoarchitectonics of molecular machines, biomolecular machines, and microrobots in their collective behaviourChemicalScienceREVIEWPublished on 29 April 2026Licensed under CC-BY 4.0NanoarchitectonKatsuhiko ArigaKPIHf2oasCaHaTaResearch Center for Materials NanoarchiteScience (NIMS), 1-1 Namiki, Tsukuba 305-nims.go.jpbGraduate School of Frontier Sciences, The UKashiwa 277-8561, JapancKey Laboratory of Multifunctional NanoInstitute of Nano-tech and Nano-bionics ((CAS), Suzhou 215123, P. R. ChinaCite this: Chem. Sci., 2026, 17, 12249Received 27th February 2026Accepted 28th April 2026DOI: 10.1039/d6sc01674jrsc.li/chemical-science© 2026 The Author(s). Published byics of molecular machines,biomolecular machines, and microrobots in theircollective behaviourKatsuhiko Ariga, *ab Wenyan Lyub and Jingwen Song*cNanoarchitectonics of small-scale molecular units into functional materials is a key strategy in materialsscience. The central challenge lies in assembling, integrating, and nanoarchitecting fundamentalfunctional units, such as molecular machines and microrobots, to innovate materials. This reviewexamines collective behaviours typical in molecular and biomolecular machines and microrobots. Wecategorize collective behaviours into six types: (i) small-scale units operating cooperatively orcollaboratively (often seen in macroscopic objects such as crystals); (ii) free-moving units in the bulkmaterial; (iii) mechanical coupling between units resulting in chain interactions (not unlike gears); (iv)assembly of units to generate macroscopic output functions; (v) macroscopic stimuli controllingindividual units; and (vi) cooperation between different molecular species to generate functional flowswithin a single system. After categorizing collective behaviours in molecular machines, we considerexamples of material systems exhibiting this behaviour, such as MOFs, COFs and crystals. Furthermore,we examine the collective behaviours of molecular machines at solid surfaces and liquid interfaces.Additionally, we highlight the behaviour of biomolecular machines and microrobots in separate sections.Each section identifies and discusses trends in the relevant examples. This approach to utilizingmolecular machines is anticipated to create highly functional systems, realizing the ultimate goal offunctional materials chemistry.atsuhiko Ariga received hishD degree from the Tokyonstitute of Technology in 1990.e joined the National Instituteor Materials Science (NIMS) in004 and is currently the leaderf the Supermolecules Groupnd a senior scientist withpecial missions of Researchentre for Materials Nano-rchitectonics (MANA), NIMS.e has also been appointed asprofessor in The University ofokyo.ctonics, National Institute for Materials0044, Japan. E-mail: ARIGA.Katsuhiko@niversity of Tokyo, 5-1-5 Kashiwa-no-ha,materials and Smart Systems, SuzhouSINANO), Chinese Academy of Sciencesthe Royal Society of ChemistryIntroductionThroughout the history of science, the development of mate-rials has preceded recognition of the signicance of structuralcontrol. Chemical sciences have signicantly expanded theavailable material repertoire.1 The emergence of nanotech-nology and nanoscience2 further transformed our ability toobserve3 and manipulate4 structures at the atomic andWenyan LyuWenyan Lyu is a PhD candidatein Professor Katsuhiko Ariga'sgroup at The University ofTokyo. Her research expertise liein interfacial cell regulation.Aer earlier work on per-uorocarbon interfaces forcontrolling cellular fate, she iscurrently developing a newgeneration of all-aqueous systeminterfaces designed to modulatecellular functions.Chem. Sci., 2026, 17, 12249–12278 | 12249http://crossmark.crossref.org/dialog/?doi=10.1039/d6sc01674j&domain=pdf&date_stamp=2026-06-26http://orcid.org/0000-0002-2445-2955https://creativecommons.org/licenses/by/4.0/Chemical Science Reviewmolecular level, unveiling still more unique properties ofnanoscale materials and the physics of nanospaces.5 Amongvarious nanoobjects, molecular machines are currently thepinnacle of research aiming to create smaller, more preciselyarchitected functional structures.6 They are dened as discretemolecules or assemblies of components designed to performmechanical, directional movements in response to specicenergy inputs. Parallelly, nanobots andmicrorobots are anothercategory of microscopic objects made of nanoparticles ormicromaterials that exhibit spontaneous propulsive motion.7Biomolecules are great bases for micromachines andmicrorobots, as demonstrated in DNA manipulation tech-nology.8 In fact, biological processes oen involve instances ofmicroscale mechanical movement driven by biomolecularmotors,9 and the implicated molecules can therefore beconsidered biomolecular machines. If we extend the denitionof mechanical manipulation to include processes such as shapetransformation, then enzymes10 and membrane channels11 arealso biomolecular machines.In short, the aim is to develop functional machine-likeobjects from molecules, nano- and micro-materials, andbiomolecules. The current challenge lies in assembling andintegrating molecular machines and microrobots to performcomplex functions in a compact form factor. Real life problemsrequire coordination of compartmentalized functions to besolved. This is most obvious in biological systems, whichcomprise multiple functional units,12 such as biomolecularmachines, working in a coordinated manner. This quintessen-tially demonstrates how smaller components can collabora-tively yield highly functional macroscopic outputs. Thiscoincides with the concept of nanoarchitectonics (Fig. 1),13which is described below.Nanoarchitectonics is dened as building functional mate-rials constructively from fundamental units,14 such as atoms,molecules and nano-objects.15 Techniques from various elds,including atomic and molecular manipulation, chemicaltransformation (such as organic synthesis), physical materialtransformation, spontaneous processes (such as self-assemblyJingwen SongJingwen Song received her PhDdegree from The University ofTokyo under the guidance ofProfessor Katsuhiko Ariga in2021. She also studied in theSupermolecules Group at theWorld Premier International(WPI) Research Centre for Mate-rials Nanoarchitectonics (MANA),National Institute for MaterialsScience (NIMS), from 2018 to2021. She then continued atNIMS as a postdoctoralresearcher in the Medical SoMatter Group from 2021 to 2025. She is currently an AssociateProfessor at the Suzhou Institute of Nano-Tech and Nano-Bionics,Chinese Academy of Sciences (SINANO, CAS).12250 | Chem. Sci., 2026, 17, 12249–12278and self-organization), orientation and organization controlusing external forces and elds, nanofabrication, micro-fabrication and biochemical processes can be combined totransform and organize the fundamental units.16 This approachcreates functional materials by leveraging the properties ofnanostructures, so its application is not limited to specicmaterials or applications. In a sense, since all matter is made upof atoms and molecules, the nanoarchitectonics methodologycan be applied to all matter. If the ultimate theory of physics isthe theory of everything,17 then nanoarchitectonics could beconsidered a method for everything in materials science.18Applying the concept of nanoarchitectonics could bea productive approach to developing molecular machines andmicrorobots. Armed with a large and varied repertoire ofnanoscale materials, as well as techniques to manipulate andobserve them at the molecular level, we are well equipped totake on the next challenge in assembling and combining theseunits to create functional materials.With the ultimate aim of creating articial systemscomprising coordinated functional units yielding remarkablefunctions in mind, this review discusses the nanoarchitectonicsof molecular machines, biomolecular machines and micro-robots. It must be noted that this topic entails many unsolvedchallenges and technologies still in their infancy, so thecollective behaviours involving the described machines may notall perfectly align with our prescribed categorization. Never-theless, we crudely envision the following categories of collec-tive behaviours: (i) units working in tandem, such as gear-likeintertwining of molecular rotors, as observed in crystallinelattices; (ii) machines moving freely within a bulk material orsubstance; (iii) ensembles of interacting molecular componentsgenerating interconnected, gear-like motions; (iv) collectiveaction of molecular machines to generate a uniedmacroscopicoutput; (v) macroscopic stimuli governing the behaviour ofindividual units within an assembly; and (vi) diverse machinetypes working within a single system to produce functionalows.Given the diversity of these behavioural patterns, this revieworganizes examples by material, system and environment,rather than by behavioural pattern alone. Nevertheless, we doexamine potential associations between materials and systemsand corresponding behavioural patterns. We rst delve into thecategories of collective behaviours we have identied, and thenwe exemplify molecular machines exhibiting such behavioursin material systems such as MOFs, COFs, and crystals. Next, weexamine collective behaviours of molecular machines on solidsurfaces and in liquid interfacial environments. Separatesections are dedicated to the distinct behaviours of biomolec-ular machines and microrobots. While the examples presentedare not exhaustive, they demonstrate the types of collectivebehaviours that can be observed in molecular machines andmicrorobots in various materials and environments.The aim of this review is to point out the way forward forcutting-edge objects such as molecular machines and micro-robots. Until now, researchers have focused on the individualoperation of molecular machines. However, the path to futurefunctional materials lies with exploring collective behaviour. As© 2026 The Author(s). Published by the Royal Society of ChemistryFig. 1 Outline of the nanoarchitectonics concept (top) and the modes of collective behaviour in molecular machines.Review Chemical Sciencethe research is gaining momentum, this review will examinetrends across material systems and environments. We explorethe paradigm shi from individual to collective behaviour,while contemplating how this property can be applied in func-tionally organized materials.Some examples of molecular machinecollective behaviour in assembliesIn this section, we will showcase the collective action ofmolecular machines within molecular and ensemble systems.Fig. 2 shows a molecular gear operating within a complexmolecule as described by Kobori, Kobayashi and co-workers.19This gear self-assembles from a 4 : 1 complex of Rh(III)Cltetrakis(4-methylphenyl)porphyrin and the bowl-shaped tetra(4-pyridyl)cavitand via axial coordination bonds between the Rh-pyridyl groups. This self-assembled complex behaves asa quadruple interlocking gear with an internal space. Thismolecular gear system comprises four connected gears. Theextremely strong porphyrin-Rh-pyridyl axial coordination bond,the rigidity of the methylene-bridged cavitand acting as a scaf-fold for the pyridyl axis, and the cruciform arrangement ofinterlocking p-tolyl groups acting as the teeth enable thismolecular assembly to function as a 14-unit gear. The cross-shaped arrangement of the four aryl groups acting as gearteeth allows the molecule to function as a quadruple inter-locking gear in solution without a sliding or rotational mecha-nism. This example demonstrates how the clever design of© 2026 The Author(s). Published by the Royal Society of Chemistrymolecular components can enable collective behaviours,whereby the molecules work together like gears.Another example of coordinated molecular motion in anassembly is the supramolecular gear. D'Agostino, Chierotti,Katrusiak and co-workers investigated the structure and solid-state dynamics of the supramolecular salt, (12-crown-4)2-$DABCO$H2O$(X)2 (where X = BF4 or ClO4, and DABCO = 1,4-diazabicyclo[2.2.2]octane).20 All components of the supramo-lecular complex demonstrate dynamic processes at roomtemperature and pressure. The crown ether motion is main-tained even at lower temperatures and higher pressures. This isbecause neighbouring molecules mesh and rotate together likehelical gears. Pressure can trigger the engagement and disen-gagement of these gears. By optimizing the molecular designand assembly structure, articial molecular rotors can exhibitcoordinated collective behaviours.Some materials are designed to exhibit excellent propertiesthrough the cooperative action of molecular machines, evenwithout direct contact. The research group led by Ito et al.developed a supramolecular gel structure boasting topologicalproperties derived from its rotaxane structure, which isfrequently employed in molecular machines (Fig. 3).21 This geldiffers from physical and chemical gels in that its crosslinks aredesigned to move freely. This gel is known as a slide-ring ortopological gel. In this gel, polymer chains with bulky endgroups are topologically connected by gure-eight crosslinksrather than covalent crosslinks (like those in chemical gels) orattractive interactions (like those in physical gels). TheseChem. Sci., 2026, 17, 12249–12278 | 12251Fig. 2 A molecular gear operating within a complex self-assembled from a 4 : 1 complex of Rh(III)Cl tetrakis(4-methylphenyl)porphyrin and thebowl-shaped tetra(4-pyridyl)cavitand via axial coordination bonds between the Rh-pyridyl groups. Reprinted with permission from ref. 19,Copyright 2016 American Chemical Society.Fig. 3 Supramolecular gel structure known as a slide-ring gel boastingtopological properties derived from its rotaxane structure, in whichpolymer chains with bulky end groups are topologically connected byfigure-eight crosslinks rather than covalent crosslinks (chemical gels)or attractive interactions (physical gels). Reprinted with permissionfrom ref. 21, Copyright 2007 Springer-Nature.Fig. 4 Mechanically interlocked semicrystalline networks containingrotaxanes, using 24-crown-8 ether as the interlocking crosslinkingagent. Incorporating mechanical chemistry into conventional semi-crystalline networks simultaneously enhances conventionally contra-dictory material properties such as mechanical toughness, strengthand elasticity. Reprinted with permission from ref. 22 Copyright 2023Wiley-VCH.Chemical Science Reviewcrosslinks can therefore move freely along the polymer chain,equalizing the tension in the polymer chain as though it werea pulley. Consequently, the gel exhibits tough mechanicalproperties. The collective action of the butyric acid molecularmachines within the gel is reected in its macroscopicproperties.The mechanical properties of materials that utilize thecollective behaviour of rotaxane molecular machines are12252 | Chem. Sci., 2026, 17, 12249–12278currently being studied in more detail. Qu and co-workersconstructed mechanically interlocked semicrystallinenetworks containing rotaxanes, using 24-crown-8 ether as theinterlocking crosslinking agent (Fig. 4).22 Incorporatingmechanical chemistry into conventional semicrystalline© 2026 The Author(s). Published by the Royal Society of ChemistryReview Chemical Sciencenetworks at once enhances conventionally contradictory mate-rial properties such as mechanical toughness, strength andelasticity. Mechanical toughness and strength result from thedissociation of crystalline domains through sieve-like macro-cycles. The nanocrystalline domains and ring-sliding effectaccelerate segmental motion and efficiently reduce energydissipation. Elastic contraction of exible segments within theamorphous polymer matrix is promoted, resulting in instanta-neous recovery.Yasuda, Mayumi, Ito and co-workers used coarse-grainedmolecular dynamics simulations to study the mechanicalbehaviour of slide-ring gels under large deformations.23 Understrain, these gels exhibit uniform chain orientation and effi-cient stress distribution through the network. When the gel isdeformed, the distribution of network strand lengths changes.During stretching, the chains reorganize into short and longsections. Slide-ring crosslinks are anchored at the ends or kinksof the polymer chains, ensuring that only the long polymerstrands remain oriented in the stretching direction (Fig. 5). Thissuppresses strain hardening at large strains and relieves stressconcentrations, providing the molecular basis for unusuallyhigh toughness in slide-ring gels.Mayumi, Ito and co-workers developed a polyethylene glycolhydrogel cross-linked with a moderate amount of polymerforming sliding rings.24 This gel uses a damage-free tougheningstrategy for hydrogels involving strain-induced crystallization.In slide-ring gels, where polyethylene glycol chains are highlyoriented and in contact with each other under large deforma-tions, crystallinity forms and melts with stretching andcontraction. The result is both rapid recovery of nearly 100% ofthe extensional energy and excellent toughness, the latter beingan order of magnitude greater than that of covalently cross-linked homogeneous polyethylene glycol gels.Fig. 5 Slide-ring gels exhibiting uniform chain orientation and efficienstrand lengths changes with deformation and the chains reorganize inCopyright 2025 Royal Society of Chemistry.© 2026 The Author(s). Published by the Royal Society of ChemistryThis section has presented some examples of cooperativeaction of molecular machines within an assembly yieldingincreased motion and impact. With appropriate design andarrangement of molecules, the rotors can interlock with eachother and act as gears. Furthermore, even without directcontact, rotaxane molecular machines located remotely cancooperate to control the properties of larger objects (such asgels) via polymer chains, achieving high performance not seenin conventional materials. Having considered assemblies ingeneral terms in this section, the next section will examine thecollective behaviour of molecular machines in structurallycontrolled materials and environments.Collective behaviour in MOF and COF nanospacesMolecular machines require molecular space within which tomove. One effective approach is to use a host material withample nanospace, which allows multiple molecular machinesto act in unison within the material. Porous materials arepromising candidates for this reason. Metal–organic frame-works (MOFs)25 and covalent organic frameworks (COFs)26 aretwo materials that full this requirement because they can beassembled while maintaining the structural precision of thenanospace. This section introduces research into the collectivebehaviour of molecular machines within MOFs and COFs.Light-driven molecular motors can drive unidirectionalrotation, and their behaviour in solution is well understood.However, Brownian motion complicates the precise nanoscalepositioning necessary to harness cooperative action. Browne,Wezenberg, Feringa and co-workers demonstrated molecularmotors organized within MOFs (Fig. 6).27 The motor units formpart of an organic linker. Light-driven, unidirectional rotationof thesemotor units is preserved within theMOF structure. Thisenables the motors to operate in the solid state at the samet stress distribution through the network. The distribution of networkto short and long sections. Reprinted with permission from ref. 23,Chem. Sci., 2026, 17, 12249–12278 | 12253Fig. 6 Molecular motors organized within MOFs, allowing them to operate at the same light-driven, unidirectional rotational speed (thermalhelix reversal speed) in the solid state as they would in solution. Reprinted with permission from ref. 27, Copyright 2019 Springer-Nature.Chemical Science Reviewrotational speed (thermal helix reversal speed) as they would insolution. The framework design ensures sufficient free volume,enabling the motor units within the pillars to perform 360°unidirectional rotation without hindrance. Potential applica-tions include gas diffusion control, directional light-drivenmass transport and miniature light-driven pumps in micro-uidic devices.In addition to enabling the free rotation of molecular rotors,the nanospace provided by MOFs can also be used to control therotation. Several studies have been conducted to validate thisidea. Feng, Xu, Tang and co-workers reported a system thatincorporates an aggregation-induced luminescent rotor ligandinto a MOF structure, known as (ZnETTB) (ETTB =40,4000,40000 0,4000000-(ethene-1,1,2,2-tetrayl)tetrakis(([1,10-biphenyl]-3,5-dicarboxylic acid))).28 The b-benzene ring in the MOFframework has minimal rotational resistance and consequentlyrotates freely under excited-state conditions. Furthermore,incorporating N,N-diethylformamide as a guest ligand inhibitsthe rotation of the b-benzene ring. This limits the effect ofintramolecular motion in the excited state, signicantlyenhancing luminescence.Fig. 7 Bicyclopentane, two types of pyridyl rotor and an azo group repenetrating pillar MOF. Adsorption of iodine vapor induces structural reapiston-like motion. Reprinted with permission from ref. 29, Copyright 2012254 | Chem. Sci., 2026, 17, 12249–12278Combiningmolecular rotors with optical functions andMOFscontaining twisted aggregation-induced luminescent rotors isuseful for sensing and detection applications. Multiple rotorsengaging in collective behaviours within the MOF enhances thesignal intensity sufficiently to meet thresholds. By engagingseveral mechanical components within the MOF, Bracco,Comotti and co-workers demonstrated that controlling thecooperative rotational motion of the MOF structure can enablethe creation of molecular machines in the solid state.29 Ina exible, double-interpenetrating pillar MOF, they organizedfast-moving components, including bicyclopentane, two types ofpyridyl rotor and an E-azo group responsible for high-precisionpedalling motion. Structural rearrangements induced by iodinevapor adsorption, for example, can displace two distinctsubnetworks through cooperative piston-like motion (Fig. 7).Such designs could lead to the development of highly sophisti-cated interlocking mechanisms for molecular machines.Various materials that incorporate molecular machinestructures into MOF structures have been reported. Forexample, Chen, Zhu and co-workers constructed MOFs usingmechanically linked [3]rotaxanes as ligands.30 Thesponsible for pedalling motion organized in a flexible, double-inter-rrangements, displacing two distinct subnetworks through cooperative24 Wiley-VCH.© 2026 The Author(s). Published by the Royal Society of ChemistryReview Chemical Sciencenanoconnement effect of the macrocyclic structure keeps theexible bis(p-phenylene) axis in a pseudo-rigid state. Coordi-nation with Zn(II) ions results in the formation of 2D and 3DMOFs. This approach of mechanically rigidifying exibleligands sheds light on MOF design. Zhai and co-workersintroduced molecular rotors into MOFs to investigate thecontrolled gate-opening effect of organic linker motors.31Introducing molecular rotors with different motional propertiesinto MOFs enhances their responsiveness, enabling precisecontrol over the recognition, adsorption and separation of gasmolecules (Fig. 8). This unique adsorption behaviour is drivenby the gate-opening effect induced by rotation of the molecularrotors. For instance, electrostatic attraction between theframework and C2H2 molecules can greatly enhance C2H2adsorption at low pressure, thereby improving C2H2 selectivity.Zhai and co-workers also demonstrated that controllable C2H2/CO2 adsorption separation can be achieved by introducingmolecular rotors to adjust the pore environment of MOFs ina purposeful manner.32 Introducing smaller ligands increasesthe pore size, providing CO2 with more opportunities to interactwith the 2D layers and strengthening its interaction with theframework, thereby enabling selective CO2 capture.MOF structures that incorporate molecular machines exhibita variety of properties. Another interesting phenomenon is theability to control the mechanical properties of MOF materialswith the collective effects of molecular machines incorporatedinto MOFs. Mei, Feng, Shi and co-workers synthesized a photo-responsive metal–organic rotaxane framework using a cucurbitFig. 8 Molecular rotors with differing motional properties introducedinto MOFs. Rotation of the molecular motors drives a gate-openingeffect, precisely modulating the adsorption and separation of gasmolecules. Reprinted with permission from ref. 31, Copyright 2024Royal Society of Chemistry.© 2026 The Author(s). Published by the Royal Society of Chemistry[8]uril-based macrocyclic pseudorotaxane linker and a photo-active styrene-derived guest molecule, (E)-4-[2-(methylpyridin-4-yl)vinyl]benzoic acid (Fig. 9).33 Due to the connement effect ofthe macrocyclic structure and the role of the columnar structurein 3D lattice stacking, the bending speed of this crystallinematerial is two orders of magnitude slower than that of otherphotoresponsive crystalline materials. Consequently, thebending motion of the crystalline state can be preciselycontrolled. This paves the way for the development of molecularmachine materials with microscopic and macroscopicdynamics, as well as stimuli-responsive behaviour. Li et al.reacted 4,40,40-triphenylamine tricarboxylate, which has a uni-que molecular rotor structure, with rare-earth metal ions toobtain dynamic luminescent MOFmaterials.34 Efficient transferof absorption energy to the rare-earth metal ions via theantenna effect resulted in emission in the blue, yellow-green,red and near-infrared regions. These luminescent propertiesare useful for sensing substances. The detection limit for Al3+ions was far below the maximum concentration specied by theUS Environmental Protection Agency for drinking water. Simi-larly, the detection limit for H2O2 was much lower than theH2O2 content in cancer cells. Furthermore, Gd(III)-containingMOFs exhibit singlet oxygen generation ability and blue ligandemission. Introducing aggregation-induced emission lumi-nogens with molecular rotor structures improves the sensingperformance of the luminescent MOFs, paving the way fordynamic, highly sensitive sensor materials.Dynamic COFs are a promising platform for so actuators.By incorporating dynamically operating molecular rotors intoCOFs, Pi and co-workers synthesized COF lms with excellentguest-dependent structural exibility and moisture-drivenactuation (Fig. 10).35 These COF lms possess intramolecularhydrogen bonds within the azine-pyridine molecular backbonethat act as specic locks, opening and closing the N–N bondedmolecular rotors in response to guest molecules. This guest-dependent structural transformation is modulated by thehydrogen bond between the pyridinyl N and guanidinium N,and integrating this COF lm into a portable respiratorymonitoring system could lead to diagnostic systems for respi-ratory diseases, such as sleep apnoea and asthma.Porous materials such as MOFs and COFs exhibit regularporosity, providing nanospaces in which molecular machinescan move freely. As the above examples demonstrate, largenumbers of molecular machines can undergo collective actionswithin these materials. This property enables precise,molecular-level properties and functions to be translated intomacro-level outputs. This is a highly rational strategy forexpressing molecular-level phenomena as macroscopic func-tions while eliminating detrimental interference betweencomponents. The collective behaviour of molecular machines inMOFs and COFs demonstrates potential as a strategy for con-verting molecular functions into practical outputs.Action within crystalsThe concept of conning molecular machines within thenanospace of MOFs while allowing them to move freely can beChem. Sci., 2026, 17, 12249–12278 | 12255Fig. 9 A photo-responsive metal–organic rotaxane framework composed of a cucurbit[8]uril-based macrocyclic pseudorotaxane linker anda photoactive styrene-derived guest molecule, (E)-4-[2-(methylpyridin-4-yl)vinyl]benzoic acid. The bending speed of this crystalline material istwo orders of magnitude slower than that of other photoresponsive crystalline materials. Reproduced under terms of the CC-BY license from ref.33, 2022 Springer-Nature.Fig. 10 COF films with guest-dependent structural flexibility and moisture-driven actuation. This is enabled by intramolecular hydrogen bondswithin the azine-pyridine molecular backbone that act as specific locks, opening and closing the N–N bonded molecular rotors in response toguest molecules. Reprinted with permission from ref. 35, Copyright 2024 Wiley-VCH.Chemical Science Reviewanalogously applied in crystals. Designing crystal structuresallows for the formation of porous MOFs and gives rise toa variety of regular structures. Considering the collectivebehaviour of molecular machines in regular structures,applying this concept to crystal structures is believed to beextremely meaningful. In this section, we will provide an over-view of research examples demonstrating the collective behav-iours of molecular machines in crystal structures.12256 | Chem. Sci., 2026, 17, 12249–12278Gladysz et al. reported a crystal structure that effects thesymmetry, connectivity and rotor function of molecular gyro-scopes (Fig. 11).36 The rotor can be either an {Fe(CO)3} group oran isoelectronic and isosteric {Fe(CO)2(NO)}+ group. The statorcomprises three spokes that span both ends of the gyroscopeaxis. Adjusting the length of the spokes tunes the rotationalbarrier of the internal rotor. Molecular systems with controlledmobility have also been integrated into liquid crystal structures.© 2026 The Author(s). Published by the Royal Society of ChemistryFig. 11 A crystal structure with symmetry, connectivity and rotor function akin to a molecular gyroscope. The stator comprises three spokes thatspan both ends of the gyroscope axis; adjusting the length of the spokes tunes the rotational barrier of the internal rotor. Reprinted withpermission from ref. 36 Copyright 2004 Wiley-VCH.Review Chemical ScienceTamaoki and co-workers developed a chiral nematic liquidcrystal containing a chiral azobenzene derivative molecularsystem that exhibits reversible EZ photoisomerization accom-panied by signicant changes in helical twisting power(Fig. 12).37 Alternating cycles of UV and visible light irradiationresult in multiple rotations of a piece of glass resting on thisliquid crystal layer in the same direction. The rotation of thepiece of glass on the liquid crystal lm is controlled by thephoto-isomerisation and orientation of the embedded chiral,photo-responsive dopant molecules. This can be viewed as thecontinuous conversion of light energy into mechanical work. Itcould contribute to the development of molecular machinesthat can convert light energy into work.Yang et al. demonstrated the feasibility of constructing a 3Dmolecular gear system (Fig. 13).38 They observed a 3DFig. 12 A chiral nematic liquid crystal containing a chiral azobenzene deraccompanied by significant changes in helical twisting power. ReprinteSociety.© 2026 The Author(s). Published by the Royal Society of Chemistrysupramolecular gear network in the green-emitting polymorphof a dialkylamino-substituted anthracene-pentiptycene p-system undergoing unusual, bifurcated polymorphic transi-tions to a yellow-emitting polymorph and a different green-emitting polymorph via 3D correlated supramolecular rota-tion. Their work has shown a correlation between crystalstructure and solid-state molecular dynamics. This demon-strates how the 3D molecular gear system can efficientlytransfer thermal energy in order to drive polymorphic transi-tions, as well as inducing uorescent chromism throughremarkable conformational and packing changes.Jin and co-workers are developing various molecularmachines that operate within a crystalline matrix. In theirreview article, ‘Rotational dynamics in crystalline molecularmachines’, they examine the relationship between solid-stateivative molecular system that exhibits reversible EZ photoisomerizationd with permission from ref. 37, Copyright 2019 American ChemicalChem. Sci., 2026, 17, 12249–12278 | 12257Fig. 13 A 3D supramolecular gear network in the green-emitting polymorph of a dialkylamino-substituted anthracene-pentiptycene p-systemundergoing unusual, bifurcated polymorphic transitions to a yellow-emitting polymorph and a different green-emitting polymorph via 3Dcorrelated supramolecular rotation. Reproduced under the terms of the CC-BY license from ref. 38, 2024 American Chemical Society.Fig. 14 A luminescent crystalline molecular rotor, in which a centralpyrazine rotor is connected by an implanted transitionmetal (Cu or Au)to an easily accessible enclosure formed by two N-heterocycliccarbenes in a discrete binuclear complex. Reprinted with permissionChemical Science Reviewmolecular rotational motion and photophysical properties,such as uorescence, phosphorescence, and chiropticalresponse.39 Advances in crystalline molecular rotors, alsoknown as solid-state molecular machines, allow for the precisemodulation of molecular dynamics and demonstrate novelapproaches to controlling photophysical behaviour. Ina perspective article titled ‘Design of molecular crystals towardscrystalline molecular machines: rotors, gears, and motors’, theyfocus on designing crystalline molecular materials that facili-tate controlled molecular motion.40 They specically mentionthree major types: rotors, gears, and motors. Most existingarchitectures are based on the dichotomy between dynamic andstatic components—namely, rotors and stators. However, thepotential for more complex and emergent behaviours to arisefrom collective dynamics and distributed activity must beexplored.Bridging the gap between molecular-level design and long-range crystalline order could open up new avenues for devel-oping molecular-based dynamic crystalline materials withengineered mechanical responses. Crystalline molecular gearsystems, in particular, give way to a new design paradigm byenabling mechanically correlated motion between multiplemolecular components. These systems exhibit synchronized orcoordinated rotational motion through interdigitated struc-tures, which can be directed and regulated by crystal packingand intermolecular forces. Examples of unidirectional rotationand photoinduced gearing suggest that directional control ispossible even in rigid crystalline environments. Integratingresponsive optical, electronic or mechanical properties andmotion will be important in developing next-generation smartmaterials. Crystalline molecular machines will enable futureapplications in adaptive photonic devices, mechanical actuatorsand energy conversion systems.Some examples of molecular rotors in different crystalstructures are presented below. Jin, Ito and co-workers reporteda novel design for a luminescent crystalline molecular rotor12258 | Chem. Sci., 2026, 17, 12249–12278(Fig. 14), in which a central pyrazine rotor is connected by animplanted transition metal (Cu or Au) to an easily accessibleenclosure formed by two N-heterocyclic carbenes in a discretebinuclear complex.41 They designed a semi-closed, encapsu-lated, bimetallic complex rotor with a concave, bulky N-heterocyclic carbene stator and an aromatic rotor that is coax-ially coordinated to the transition metal along the rotation axis.This design enables the molecular rotor to rotate within thecrystal. Furthermore, the activation energy of rotation can beadjusted by altering the implanted metal. The packing structureeffect, which is oen important in many amphiphilic molecularcrystals, is absent. Based on the examples presented here,a general method can be developed that uses abundant ligandsas functional stators and metal–ligand coordination bonds astuneable rotation axes in amphiphilic crystals. This wouldgreatly facilitate the development of new functional materialsbased on changes in molecular dynamics in static crystallinesolids. Additionally, Ito, Jin and co-workers demonstrated thefrom ref. 41, Copyright 2021 American Chemical Society.© 2026 The Author(s). Published by the Royal Society of ChemistryReview Chemical Sciencesolid-state rotational motion of two larger molecules (triptyceneand pentiptycene) by encapsulating bulky N-heterocyclic car-bene Au(I) complexes in crystalline media.42 This enablesfurther study and design of systems in which large, complexmolecular units can perform rotational motion while main-taining the structural integrity of the system and the mobility ofits components.Jin and his team developed a new structural motif forluminescent, chiral, crystalline molecular rotors that exhibitchiroptical properties correlated with rotational motion incrystalline media (Fig. 15).43 By incorporating a bulky chiral capinto triaryltriazine, the chiroptical properties became correlatedwith rotational motion in the crystalline state. These stericrotors exhibit remarkable circularly polarized uorescence,which is induced by the suppression of molecular motion in anexcited state with a sterically constrained lattice environment.The bulky chiral cap was obtained by introducing a tri-isopropylsilyl group into the axially chiral binaphthyl group.Molecular rotation promotes the structural relaxation of thebulky, chiral-capped triaryltriazine in the excited state uponlight absorption. Furthermore, phenylene rotation in the crystalenhances efficient intersystem crossing through the formationof a stable triplet state. These results demonstrate a usefulmolecular design for modulating solid-state chiroptical prop-erties through rotational motion. It may be possible to tune theenergy gap between the singlet and triplet states, which isgenerally considered difficult to achieve in crystalline media.Jin, Hayashi, Rodŕıguez-Molina and co-workers createdbinary optical waveguiding crystals featuring large anisotropyand uorinated acceptor molecules with in-plane rotationaldynamics (Fig. 16).44 The charge transfer co-crystal exhibitsanisotropy due to the orientation of the transition dipolemoment, as well as high reabsorption due to crystal packing.Notably, the substantial linear increase in photoluminescenceat low temperatures can be attributed to a reduction in in-planerotational motion at these temperatures. These ndings suggestthat the co-crystal possesses excellent binary optical wave-guiding properties and thermally driven photoluminescence,making it suitable for use in optically controlled gates, forexample.Fig. 15 Chiroptical properties correlated with rotational motion in cryaryltriazine. Reprinted with permission from ref. 43, Copyright 2024 Am© 2026 The Author(s). Published by the Royal Society of ChemistryTo demonstrate gear-shi functionality at the molecularlevel, Jin, Ito and co-workers investigated a columnar, stackedclutch structure formed in the crystalline phase by a tri-aryltriazine rotor bearing bulky silane groups in the para-posi-tion of the peripheral phenylene groups (Fig. 17).45 Thecrystalline rotor's phenylene units can perform two distinct,interconvertible, correlated molecular motions. These inter-molecular rotational motions can be switched via a thermallyinduced phase transition between the crystals. The intermo-lecular stacking of C3-symmetric rotors, driven by the stericrepulsion of the bulky stator, is a promising strategy forgenerating various correlated molecular motions in the crys-talline phase. Reversible modulation of these correlated rota-tions is achieved via a thermally induced inter-crystalline phasetransition. This can function as a gear shi at the molecularlevel.Unlike MOFs, crystal structures do not provide nanospace;however, they do provide an ordered structure in whichmolecular machines can perform collective behaviours. Thesestructures allow molecular machines to move freely and cancreate systems in which multiple machines work together. It isalso noteworthy that materials can be constructed in whichmolecular gear structures, comprising interlocking molecularrotors, can be integrated. This allows movement at the molec-ular level to inuence the properties of macroscopic materials,and further advancements in this strategy are anticipated.Collective behaviour on solid surfacesAlthough many techniques exist for analysing the behaviour ofmolecular machines, the most direct method is to visualizethem through molecular imaging. These analyses are typicallyperformed using either scanning tunnelling microscopy (STM)or atomic force microscopy (AFM).46 This is achieved by placingthe molecular machine on a solid substrate. In this section, wepresent examples of research into the behaviour of molecularmotors and their associated gears at solid interfaces.As demonstrated through the examples of MOFs and crystalsmentioned above, deliberate molecular design can enablemolecular machines to function independently within thinlms on solid substrates. Kaleta et al. fabricated a monolayerstalline media achieved by incorporating a bulky chiral cap into tri-erican Chemical Society.Chem. Sci., 2026, 17, 12249–12278 | 12259Fig. 16 Optical waveguiding crystals featuring large anisotropy and fluorinated acceptor molecules with in-plane rotational dynamics where thecharge transfer co-crystal exhibits anisotropy due to the orientation of the transition dipole moment, as well as high reabsorption due to crystalpacking. Reproduced under the terms of the CC-BY license from ref. 44, 2025 American Chemical Society.Fig. 17 Stacked clutch structure formed in the crystalline phase by a triaryltriazine rotor bearing bulky silane groups in the para-position of theperipheral phenylene groups. The crystalline rotor's phenylene units can perform two distinct, interconvertible, correlated molecular motions.Reprinted with permission from ref. 45, Copyright 2023 American Chemical Society.Chemical Science Reviewsystem of optically switched rod-like molecules incorporatinga diarylethene-based switch and a unidirectional, light-drivenmolecular motor on a solid substrate (Fig. 18).47 This systemis built on a triptycene-based molecular pedestal. The lm wasthen smoothly transferred onto gold and quartz surfaces usingthe Langmuir–Blodgett (LB) technique. Repeated depositionyielded bilayer systems containing one layer with a di-arylethene-based optical switch and another with a unidirec-tional, light-driven molecular motor. It was conrmed that theoptically switched molecular machine maintained full func-tionality while operating at the solid–gas interface. By usingappropriate monochromatic light, layers composed of the sametype of optical switch can be selectively targeted. This couldpotentially be utilized to construct new types of memory devicesboasting molecular level multilayer structures.Additionally, Kaleta et al. synthesized two light-drivenmolecular motors fused to a triptycene-based tetrapodal plat-form, with their rotational axes oriented either parallel orperpendicular to the surface (Fig. 19).48 Even when assembled asmonolayers on gold surfaces, the motors maintained full12260 | Chem. Sci., 2026, 17, 12249–12278rotational functionality, demonstrating the tetrapodal plat-form's ability to minimize surface interactions. This shows thatthe tetrapodal platform effectively decouples the chromophorefrom the metal surface, making it a promising candidate fordeveloping advanced surface-mounted molecular machines.Chiral molecules have recently attracted renewed attentionas a highly efficient source of spin-selective charge release,resulting from a phenomenon known as ‘chiral-induced spinselectivity’. Noting this, Sato, Yamamoto and co-workersdeveloped self-assembled monolayers of molecular motorsbased on overcrowded alkenes (Fig. 20).49 By forming covalentbonds between electrodes and the molecules, their chirality canbe switched, allowing the direction of spin polarization to bemanipulated externally with remarkable stability and repeat-able control. Thiol-terminated alkyl chains (C8) provide thenecessary space for the structure to rotate unidirectionally.Researchers have also attempted to design molecular gearsthat intermesh with molecular rotors via attractive van derWaals interfaces, which are essential for forming highly orderedassemblies. Rapenne and co-workers designed and synthesized© 2026 The Author(s). Published by the Royal Society of ChemistryFig. 18 A monolayer system of optically switched rod-like molecules incorporating a diarylethene-based switch and a unidirectional, light-driven molecular motor on a solid substrate built on a triptycene-based molecular pedestal. Reprinted with permission from ref. 47, Copyright2024 Wiley-VCH.Fig. 19 Two light-driven molecular motors fused to a triptycene-based tetrapodal platform, with their rotational axes oriented either parallel orperpendicular to the surface. Even when assembled as monolayers on gold surfaces, the motors maintained full rotational functionality,demonstrating the tetrapodal platform's ability to minimize surface interactions. Reproduced under the terms of the CC-BY license from ref. 48,2026 Wiley-VCH.Review Chemical Sciencea ruthenium-based molecular gear consisting of a tripodalligand with a pentaphenylcyclopentadienyl ligand anchor andaryl-extended indazole teeth (Fig. 21).50 The single-crystalstructure of the ruthenium complex reveals that the appendedaryl groups increase the apparent diameter of the gear, makingit larger than the anchor unit. Consequently, when the complexadsorbs to a surface, intermolecular gearing motion becomesfavourable. The linear arrangement of the complex's tripodalligands appears to interdigitate, providing efficient propagationof rotational motion.Some studies have observed the motion of interlockingmolecular gears and molecular rotors. To realize a moleculargear train operating at the tip of an STM, each molecule must bestably anchored to a metal surface. In the case of the moleculargears demonstrated by Moresco et al., placing a tert-butyl groupon the end of one gear tooth was benecial for both tip-induced© 2026 The Author(s). Published by the Royal Society of Chemistrymanipulation and rotation monitoring.51 Using this optimizedmolecule, they achieved reproducible, stepwise rotation ofindividual gears and transmitted rotation to up to three inter-locking units (Fig. 22). Manipulating the tert-butyl tooth of onegear with the STM tip enabled them to induce steps in therotational transmission between three interlocking gears.Counterclockwise rotation of the driver caused the rst followerto rotate clockwise by 75°, while simultaneously causinganother follower to rotate counterclockwise by 78°, for a total of104°. In the aermath of a rotation step, small lateraldisplacements were observed in all three gears. The ability tocontrol the rotation of multiple gears within a gear train iscrucial for the development of molecular machines, such asmechanical computers.Van Hove and co-workers explored the transmission ofrotational motion and energy over longer distances throughChem. Sci., 2026, 17, 12249–12278 | 12261Fig. 20 Self-assembled monolayers of molecular motors based on overcrowded alkenes. The chirality of the molecules can be switched byforming covalent bonds between the molecules and electrodes, allowing the direction of spin polarization to be manipulated externally withremarkable stability and repeatable control. Reprinted with permission from ref. 49, Copyright 2023 Wiley-VCH.Fig. 21 A ruthenium-based molecular gear consisting of a tripodalligand with a pentaphenylcyclopentadienyl ligand as the anchor andaryl-extended indazole as the teeth. Reproduced under the terms ofthe CC-BY license from ref. 50, 2023 Wiley-VCH.Fig. 22 Manipulating the tert-butyl tooth of one gear with the STM tipinduces steps in the rotational transmission between three interlockinggears. Small lateral displacements were observed in all three gears perrotational step. Reprinted with permission from ref. 51, Copyright 2020American Chemical Society.Chemical Science Reviewchains of passive, gear-like ‘slave’ molecules (Fig. 23).52Ensuring that the slave molecules are fully relaxed at eachimposed driver rotation angle enables them to follow energy-optimized paths involving rotation, tilting, bending, slidingand disassembly. The quasi-classical picture of these rotationsis realistic and intuitive at a qualitative level. Therefore, neitherprediction of the general behaviour of gear rotations nor gearcouplings require quantum mechanics. Nevertheless, quantumeffects, such as the height of rotational and translationalbarriers, underlie these motions at a quantitative level.Quantum tunnelling, thermal effects and energy dissipationalso play a signicant role. This research will aid the design ofgear systems and contribute to the development of nanoscalemolecular robots.12262 | Chem. Sci., 2026, 17, 12249–12278The collective action of molecular machines on solidsurfaces can be employed to control larger, more sophisticatedmaterial systems. For instance, cell differentiation can beregulated through the collective activity of molecular machines.Feringa, van Rijn and co-workers demonstrated that thecollective dynamic motion of a layer of articial rotary molec-ular motors to UV light can inactivate adsorbed protein layers ata biological level. Since stem cells on dynamically alteredsurfaces are more likely to differentiate into osteoblasts thanthose on static surfaces, this ultimately determines the fate ofhuman bone marrow-derived mesenchymal stem cells (hBM-MSCs) (Fig. 24).53 Surfaces on which molecular motors engagein collective behaviours offer various opportunities formechanical stimulation, controlling cell fate, and creating© 2026 The Author(s). Published by the Royal Society of ChemistryFig. 23 Transmission of rotational motion and energy over longer distances through chains of passive, gear-like ‘slave’molecules. Ensuring thatthe slave molecules are fully relaxed at each imposed driver rotation angle enables them to follow energy-optimized paths involving rotation,tilting, bending, sliding and disassembly. Reprinted with permission from ref. 52, Copyright 2018 American Chemical Society.Fig. 24 Artificial rotary molecular motors on a solid surface can exert motion to control adsorbed protein layers, ultimately determining the fateof human bone marrow-derived mesenchymal stem cells (hBM-MSCs). Reprinted with permission from ref. 53, Copyright 2020 AmericanAssociation for the Advancement of Science.Review Chemical Scienceresponsive biomimetic materials. This paves the way forsynthetic molecular motors to be used in biomedical and clin-ical applications.In summary, the shape and movement of molecularmachines can be directly observed on solid surfaces. Moleculargears in which molecular rotors intertwine and move in unisonas part of a sophisticated collective behaviour have beendemonstrated. By observing molecular structures using STMand performing theoretical calculations, it is also possible tostudy the operating behaviour of molecular machines at thequantum level. Of particular note is how cell fate can becontrolled by the collective rotation of molecular motors onsurfaces. This aligns with the previously discovered paradigm© 2026 The Author(s). Published by the Royal Society of Chemistrywhereby cells receive stimuli from surfaces and undergo variouschanges. Surfaces and other environments bridge molecularmachine movement with macroscopic phenomena.Collective behaviour at liquid interfacesThe nal example in the previous section demonstrated thatinterfacial environments are ideal for integrating the operationof molecular machines with macroscopic functions. Thisproperty is particularly pronounced at liquid interfaces, wherethe interface itself is dynamic. For instance, a monolayer at theair–water interface has macroscopic dimensions in the in-planedirection, juxtaposed by its nanomolecular thickness. In suchan environment, macroscopic perturbations applied in the in-Chem. Sci., 2026, 17, 12249–12278 | 12263Fig. 25 A steroid cyclophane molecular machine with a central ring structure of cyclophane and four rigid plate-like steroid moieties to graspand capture guest molecules upon compression of its monolayer at the liquid interface.Chemical Science Reviewplane direction can be linked to molecular functions within thethickness of the lm. Thus, macroscopic behaviour and nano-scale functions can be linked at the liquid interface.54 Inte-grating molecular machines as a monolayer at the air–waterinterface makes it possible to control their collective behaviourthrough macroscopic manipulation.55The rst molecular machine to be driven through macro-scopic mechanical manipulation was a steroid cyclophane(Fig. 25).56 This machine consists of a central ring structure, orcyclophane, to which four rigid, plate-like steroid moieties areconnected via exible spacers. When compressed laterally toreduce its molecular area, this monolayer forms a cavity-likestructure. Using this property, the molecular machine cangrasp and capture guest molecules. Mechanical displacementsof several tens of centimetres induce structural changes in themolecular machine at the nanometre level, enabling exiblecontrol over the capture and release of molecules. This processcan be used to ne-tune the structure of molecular receptors.A cholesterol-armed cyclen with an asymmetric centre thatcan alter its environment by twisting was used as a molecularreceptor at the air–water interface (Fig. 26).57 The monolayerwas then compressed gradually, and recognition of chiralamino acids at various surface pressures was tested. ForFig. 26 A cholesterol-armed cyclen with an asymmetric centre that canrecognition of chiral amino acids with various surface pressures at the a12264 | Chem. Sci., 2026, 17, 12249–12278example, when valine is used as a guest molecule, the D-isomeris recognized preferentially at low surface pressure; however,this preference reverses at high surface pressure, favouring theL-isomer instead. In other words, adjusting the conformation ofthe receptor molecule at the interface can reverse the chiralselectivity, even when using the same receptor molecule.Similar tuning of molecular recognition properties has alsobeen demonstrated in the recognition of nucleobases. In thiscase, cyclononane molecules containing multiple carbonyl andtertiary amino groups are arranged on the water surface andgradually deformed by pressure in order to adjust the hydrogen-bonding structure (Fig. 27).58 Despite the structural differencebetween uracil and thymine derivatives being merely a singlemethyl group, recognition was achieved at a rate 70- to 80-foldhigher under the same conditions. This is impressive as evennucleic acids such as DNA and RNA fail to distinguish betweenthymine and uracil. Mechanical tuning is a very useful tool tond optimal structures for molecular recognition at interfaces.Molecular motors are susceptible to thermal uctuations atliquid interfaces due to their small size, which limits theirability to exert useful functions. Instead, a more feasiblestrategy is to condense molecular motors into so, orderedphases (such as liquid crystals), achieving functionality throughalter its environment by twisting was used as a molecular receptor forir–water interface.© 2026 The Author(s). Published by the Royal Society of ChemistryFig. 27 Cyclononane molecules containing multiple carbonyl and tertiary amino groups arranged on the water surface with the capability todiscriminate between uracil and thymine derivatives at the air–water interface.Review Chemical Sciencecollective molecular driving. Tabe and Yokoyama demonstratedthat a chiral liquid crystal monolayer spread on a glycerolsurface functions as a condensed layer of molecular rotorsundergoing coherent precession, driven by the movement ofwater molecules across the membrane (Fig. 28).59 This mono-layer consists of simple, rod-shaped molecules with chiralpropellers and exhibits a spatiotemporal pattern of molecularorientation that closely resembles the ‘target pattern’ observedin the Belousov–Zhabotinsky reaction. Reversing either themolecular chirality or the direction of water molecule move-ment can reverse the rotational direction of the transition froman expanding to a converging target pattern. Although therotational motion of a single molecular motor is likely to beoverwhelmed by thermal noise, the collective, cooperativemotion of molecular motors, enabled by liquid crystal ordering,has been shown to amplify tiny individual motions intomacroscale motion.As observed in crystals, the degree of rotational freedom ofmolecular rotors is dependent on the available free space. Inmonolayers on water surfaces and their collapsed three-dimensional structures, the rotational behaviour of molecularrotors depends on the packing of molecular aggregates. FromFig. 28 A monolayer of simple, rod-shaped molecules with chiral propethat closely resembles the target pattern observed in the Belousov–ZCopyright 2003 Springer-Nature.© 2026 The Author(s). Published by the Royal Society of Chemistrythis perspective, the behaviour of a 9-(2-carboxy-2-cyanovinyl)julolidine derivative, as a twisted intramolecular charge trans-fer molecular rotor, was investigated using in situ uorescencespectroscopy (Fig. 29).60 This research examined the intra-molecular rotation of molecules within 2D and 3D collapsedmonolayers at the air–water interface. In solution, this molec-ular rotor exhibited suppressed molecular rotation andincreased uorescence intensity with increasing solventviscosity. In contrast, monomer emission from the monolayerwas weaker, suggesting that intramolecular rotation is notsuppressed, even in densely ordered monolayers. Furthermore,uorescence spectroscopy of Langmuir–Blodgett (LB) lmsrevealed that molecular rotation remains unaffected even whenmonolayers are transferred to solid substrates. However, exci-mer emission due to aggregation was observed when themonolayer collapsed into a disordered 3D structure. If a 2Dordered structure can be maintained in a so aggregate ratherthan a crystal, sufficient free space will be available to enablecollective behaviour of the molecular rotors.The air–water interface is a boundary between two mediawith a large difference in dielectric constant. Consequently,these media can exhibit signicant differences in physicalllers (left) exhibiting a spatiotemporal pattern of molecular orientationhabotinsky reaction (right). Reprinted with permission from ref. 59,Chem. Sci., 2026, 17, 12249–12278 | 12265Fig. 29 Behaviours of a 9-(2-carboxy-2-cyanovinyl)julolidine derivative, as a twisted intramolecular charge transfer molecular rotor. Theintramolecular rotation of this molecular rotor is different as part of 2D and 3D collapsed monolayers at the air–water interface. Reprinted withpermission from ref. 60, Copyright 2018 Royal Society of Chemistry.Chemical Science Reviewproperties, especially engineering properties. Therefore, differ-ences in molecular conformation and orientation can result inmolecular machine-like functions. Fig. 30 shows an example ofthis, depicting the orientation and luminescence properties ofa double-paddle dinuclear PtII complex containing pyrazolerings linked by an alkyl spacer being dynamically manipulatedat the air–water interface.61 During mechanical compression,the complex emerges from water, simultaneously changing theorientation of the PtII complex planes from perpendicular toparallel and exhibiting a unique ‘submarine luminescence’effect. The complex's phosphorescence is quenched at the air–water interface before monolayer formation; then, the intensityincreases rapidly duringmonolayer compression. In submergedmode, the H-shaped dinuclear PtII complex sinks in water,resulting in weak luminescence expression due to hydrogenFig. 30 Orientation and luminescence properties of a double-paddle dinwhich are dynamically manipulated at the air–water interface. MonolaReprinted with permission from ref. 61, Copyright 2020 Wiley-VCH.12266 | Chem. Sci., 2026, 17, 12249–12278bonding. Mechanical compression then pushes the H-shapedcomplex to the surface, triggering transition to the oatingmode where the PtII complex planes behave independently atthe air–water interface. The surface in the air phase is unaf-fected by the dispersion of excitation energy due to molecularcontact in the water phase. In other words, this molecularmonolayer behaves as an assembly of molecular submarines.The operational characteristics of molecular machines thatare collectively driven at the air–water interface have also beeninvestigated. One topic of discussion has been the conversion ofmechanical energy. To this end, molecular pliers were used astheir movement is easy to assess and evaluate (Fig. 31).62Binaphthyl-type amphiphilic molecules were used as openablemolecular pliers to examine patterns in macroscopic mechan-ical energy expenditure to produce molecular deformation.uclear PtII complex containing pyrazole rings linked by an alkyl spacer,yer compression triggers a unique ‘submarine luminescence’ effect.© 2026 The Author(s). Published by the Royal Society of ChemistryFig. 31 Binaphthyl-type amphiphilic molecules used as openable molecular pliers to examine patterns in macroscopic mechanical energyexpenditure for molecular deformation. The pliers were arranged at the air–water interface and gradually compressed, and correlated with themeasured dihedral angle of the binaphthyl group. Reprinted with permission from ref. 62, Copyright 2015 Wiley-VCH.Review Chemical ScienceFirst, the pliers were arranged at the air–water interface andgradually compressed, and the dihedral angle of the binaphthylgroup wasmeasured. Based on this data, the energy required formolecular deformation was calculated using quantum chemicalmodelling. Furthermore, the energy involved in the mechanicaldeformation of a macroscopic monolayer was estimated ther-modynamically. The two values were very similar. As surfacepressure increases from 0 to 10 mN m−1, approximately0.2 kcal mol−1 of mechanical energy is stored and the sameamount of molecular deformation energy is used. In contrast, athigher pressures, the molecular deformation energy becomessmaller than the mechanical energy stored. This suggests thatmacroscopic mechanical energy can be used to very efficientlydeform molecular machines in interfacial systems.Treating molecular machines as assemblies enables modu-lation of their behaviour. The open/closed state of themolecularFig. 32 Binaphthyl derivatives, previously used as molecular pliers becaumonolayer compression, are converted to exhibit digital behaviour. Thimatrix, exploiting its phase transitions induced bymechanical stress to acof left- and right-handed helical structures), resulting in digital opening a63, Copyright 2017 Wiley-VCH.© 2026 The Author(s). Published by the Royal Society of Chemistrypliers described above is an analogue transformation inducedby monolayer compression. Alternatively, discontinuous, digitalbehaviour can be induced in the molecular pliers by placingthem in amonolayer matrix and exploiting its phase changes. Inthe mixed monolayer system shown in Fig. 32, phase transitionsinduced by mechanical stress enable the digital opening andclosing of simple binaphthyl molecular pliers.63 By applyingmechanical force at the air–water interface, phase transitions inthe monolayer matrix between a homogeneous liquid state anda metastable nanocrystalline state lead to reversible cisoid–transoid conformational transitions (i.e., reversal of le- andright-handed helical structures) of binaphthyl derivatives. Sincethe conformational change is reversible, repeated crystalliza-tion and dissolution of metastable binaphthyl crystals inducesrepeatable alteration of the binaphthyl assembly's molecularstructure. Thus, digital opening and closing of the molecularse they natively exhibit analogue transformation behaviour induced bys is accomplished by placing the binaphthyl derivative in a monolayertivate reversible cisoid–transoid conformational transitions (i.e. reversalnd closing of the molecular pliers. Reprinted with permission from ref.Chem. Sci., 2026, 17, 12249–12278 | 12267Chemical Science Reviewpliers can be realized through external mechanical stimulationat the air–water interface.The air–water interface is an ideal medium for controllingthe assembly of molecules and the clustering of molecularmachines. Maaloum, Semenov, Giuseppone and co-workersreported supramolecular polymerization at the air–water inter-face induced by the rotation of molecular motors (Fig. 33).64Providing the system with an appropriate energy source, such asphotons, enables the autonomous, non-equilibrium motion ofthe monomers to be manipulated, thereby controlling thepolymer structure and altering its growth dynamics. On average,the motors maintain a stable state, and the mechanical workgenerated by the photo-stimulated rotation of individualmotors drives the formation and growth of nanostructures. Thisclustering phenomenon, which is controlled by precise andrapid nanomechanical motion, is conceptually distinct fromthermal annealing processes. Unlike non-specic heatingprocesses, the motion is conned to the driving parts of themolecular motors. This approach could lead to new ways ofcontrolling so matter at the nanoscale.Macroscopic mechanical actions and molecular motions canbe coupled at the air–water interface. Integrating molecularmachines at this interface enables them to be driven bymacroscopic mechanical stimuli and optimizes the function ofmolecular receptors. Furthermore, the efficiency of macro-scopic energy consumption to drive molecular machines isFig. 33 Supramolecular polymerization at the air–water interface inducwork generated by the rotation of individual motors drives the formationCopyright 2025 Springer-Nature.12268 | Chem. Sci., 2026, 17, 12249–12278extremely high. Despite its so structure, the monolayer at theair–water interface secures free space that ensures the collectivemotion of molecular rotors and other molecules. At the air–water interface, collective properties, such as phase separationand supramolecular polymerization, can be adapted to drive thefunctions of molecular machines. The strategy of using molec-ular machines at liquid interfaces, most notably the air–waterinterface, has great potential to open up new scientic frontiers.Collective behaviour of biomolecular machinesBiological systems exhibit far more sophisticated functionsthan articial supramolecular systems. They are home tonumerous biomolecular machines, the most sophisticated andfunctional of which are proteins. Harvesting these biomolecularmachines and articially organizing them to function collec-tively is a promising approach for developing advanced func-tional systems. Some examples utilizing this strategy areintroduced in the following sections.The rst example illustrates a method for creating nano-pores with sophisticated machine capabilities via proteinassembly. Maglia et al. engineered an integrated multiproteincomplex that controls the unfolding and transport of individualproteins through a nanopore (Fig. 34).65 Replacing proteinsurface loops with the membrane-spanning region of a b-barrelpore, anked by short hydrophilic linkers, enables cyclic,soluble proteins to be inserted into lipid membranes. Using thised by photo-stimulated rotation of molecular motors; the mechanicaland growth of nanostructures. Reprinted with permission from ref. 64,© 2026 The Author(s). Published by the Royal Society of ChemistryFig. 34 An integrated multiprotein complex that controls the unfolding and transport of individual proteins through a nanopore. Reprinted withpermission from ref. 65, Copyright 2021 Springer-Nature.Review Chemical Sciencemethodology, the archaeal 20S proteasome was incorporatedinto an articial nanopore to control the unfolding and lineartransport of proteins through the nanopore. Selected substrateproteins are unfolded and delivered to the proteasome chamberfor processing into fragmented peptides or intact polypeptides.This enables new approaches for analysing proteins at theFig. 35 A methodology for the self-assembly of highly ordered, electricDNA nippers. The high local concentration of nippers organized on homnanomachines, boasting improved translocation efficiency over conveCopyright 2018 American Chemical Society.© 2026 The Author(s). Published by the Royal Society of Chemistrysingle-molecule level, à la protein sequencing. The nanoporecould function as a stable, low-noise b-barrel nanopore sensor.Yuan, Zhuo, Chai and co-workers demonstrated a method-ology for the self-assembly of highly ordered, electric-eld-free3D DNA nanostructures using azobenzene-functionalized DNAnippers (Fig. 35).66 The high local concentration of nippers-field-free 3D DNA nanostructures using azobenzene-functionalizedogeneous DNA nanostructures enables them to function as 3D DNAntional 3D nanomachines. Reprinted with permission from ref. 66,Chem. Sci., 2026, 17, 12249–12278 | 12269Chemical Science Revieworganized on homogeneous DNA nanostructures enables themto function as 3D DNA nanomachines with improved trans-location efficiency over conventional ones. Incorporating azo-benzene moieties into the DNA nippers preserves thenanostructure of the DNA nanomachine and enables thereversal of nanomachine translocation in a single, rapid step. Inthe presence of a target microRNA (miRNA), hybridizationbetween the miRNA and the nipper generates an open state,reected by an enhanced electrochemiluminescence (ECL)signal from Ru(bpy)22+ due to its proximity to the Alexa Fluorquencher. This method can be applied in rapid, single-stepdetection of biomarkers, with applications in sensing, anal-ysis, and diagnostics. Cancer-cell-derived biomarkers can beanalysed quantitatively with ultra-high sensitivity in a rapidsingle step process. This could provide a route to next-generation nanomachines for early cancer detection anddiagnosis.Collectively operating synthetic DNA machines on nanoscale3D tracks are rapidly gaining attention due to their potentialapplications in areas such as biocomputing, drug delivery andbiosensing. Yang, He and co-workers were the rst to reportspatially separated 3D DNA tracks based on polyadenine (polyA)(Fig. 36).67 They developed a walking device consisting ofa target-activated DNAzyme walker and the 3D track adsorbedonto an AuNP surface via polyA. The DNAzyme walker movesalong this track via a burnt-bridgemechanism, through which itdemonstrates improved efficiency and throughput. TheDNAzyme-walking-device-based sensor demonstrated cascadesignal amplication resulting in selective and sensitive detec-tion of adenosine, Ag+, and target DNA. This demonstrates greatpotential in high-performance, bioinspired DNAnanomachines.Fig. 36 Spatially separated 3D DNA tracks adsorbed onto AuNPs via polmolecules form a sensor that sensitively and selectively detects adenCopyright 2018 American Chemical Society.12270 | Chem. Sci., 2026, 17, 12249–12278Current systems oen rely on manual application of externalstimuli, which limits the potential of autonomous molecularsystems. In a breakthrough, Kakugo, Nomura and co-workersdemonstrated that a DNA-based cascade reaction can functionas a molecular controller, driving the autonomous assemblyand disassembly of DNA-functionalized microtubules via kine-sin (Fig. 37).68 The system comprises three DNA complexes andthree enzymes, referred to as the template, converter, andtransducer. The three enzymes, a polymerase, nickase andrestriction enzyme, can synthesize new DNA from templateDNA, cleave half of a double-stranded DNA and completelycleave double-stranded DNA, respectively. By designing a reac-tion cascade consisting of cDNA hybridization, DNA stranddisplacement, and enzyme activity, the molecular controller canautonomously execute each step of the cascade. Glidingmicrotubules integrated into the controller assemble intobundled structures and disassemble into individual lamentsin the absence of any external stimuli. This introduces a newconcept of autonomously controlled materials driven by mole-cules and equipped with a smart controller that encodes thesystem's instructions.Jia et al. reported a system in which glyceraldehyde-3-phosphate dehydrogenase (GAPDH), 3-phosphoglyceratekinase (PGK), formate dehydrogenase (FDH) and ATPase-incorporated proteoliposomes were co-immobilized usinghollow polydopamine (HPDA) as a biocompatible scaffold(Fig. 38).69 Within this microreactor, GAPDH and PGK catalysethe conversion of glyceraldehyde-3-phosphate to 3-phospho-glycerate, reducing b-nicotinamide adenine dinucleotide(NAD+) to NADH and generating a proton inux to drive ATPsynthesis. The microreactor exhibits a strong affinity for CO2,a property exploited with the aid of FDH to facilitate theyadenine (polyA), and a target-initiated DNAzyme walker; together theosine, Ag+, and target DNA. Reprinted with permission from ref. 67,© 2026 The Author(s). Published by the Royal Society of ChemistryFig. 37 A DNA-based cascade reaction functioning as a molecular controller, driving the autonomous assembly and disassembly of DNA-functionalized microtubules via kinesin. The system comprises three DNA complexes and three enzymes to autonomously execute each step ofthe cascade, in the absence of any external stimuli. Reproduced under the terms of the CC-BY license from ref. 68, 2024 American Associationfor the Advancement of Science.Review Chemical Sciencereduction of CO2 to formate and the oxidation of NADH toNAD+, enabling recycling of the NAD+/NADH redox couple. Thisprocess also supplies protons to drive ATP production. ThisFig. 38 Co-immobilization of glyceraldehyde-3-phosphate dehy-drogenase (GAPDH), 3-phosphoglycerate kinase (PGK), formatedehydrogenase (FDH) and ATPase-incorporated proteoliposomes onhollow polydopamine (HPDA), which serves as a biocompatible scaf-fold. This creates a microreactor, wherein GAPDH and PGK catalysethe conversion of glyceraldehyde-3-phosphate to 3-phosphoglyc-erate, reducing b-nicotinamide adenine dinucleotide (NAD+) to NADHand generating a proton influx to drive ATP synthesis. The micro-reactor has a strong affinity for CO2, a property exploited with the aidof FDH to reduce CO2 to formate and oxidize NADH to NAD+, recy-cling the NAD+/NADH redox couple for efficient energy synthesis fromlow-value substrates. Reprinted with permission from ref. 69, Copy-right 2025 Wiley-VCH.© 2026 The Author(s). Published by the Royal Society of Chemistrynanoarchitectonic microreactor expertly coordinates bothchloroplast and mitochondrial enzymes, essentially recreatingthe functional coordination of these organelles in vitro. Weanticipate that this approach will inspire methods for moreefficient ATP synthesis from low-value substrates, with potentialto address environmental and energy challenges.Fei, Li and co-workers constructed a compartmentalizednanostructure to regulate bioenergetic levels (Fig. 39).70 In theassembled structure, glucose dehydrogenase (GDH), urease andnicotinamide adenine dinucleotide were encapsulated byliquid–liquid phase separation. ATPase and glucose trans-porters embedded in hybrid liposomes were attached to thecapsule surface. In this nanostructure, glucose is transportedand converted to gluconate by GDH, creating an outward protongradient to drive ATP synthesis. In parallel, urease catalysed thehydrolysis of urea to produce ammonia, creating an inwardproton gradient to drive ATPase for ATP decomposition. Theseprocesses alter the direction of the proton gradient, resulting inarticial ATP oscillations. The frequency and amplitude of theseoscillations can be precisely tuned by varying the loading of theencapsulated enzymes and the fuel concentrations (glucose andurea) within the nanostructure. This design innovates a newstrategy for developing nanoarchitectures that can controlbioenergetics levels in opposing directions.The systems described above highlight howmultiple types ofbiomolecular machines can work in concert. These biomolec-ular machines are not limited to collective action of singularmolecular species; there are also systems of diverse biomolec-ular machines collaborating. A major advantage of biomolec-ular machine assemblies is that they excel at coordination ofdiverse molecular machines serving different functions withinthe system, creating a ow of function. Biomolecular machineshave sophisticated and highly functional capabilities, and theircoordinated action can yield functions rivalling or evensurpassing those of living organisms. Developing host materialsChem. Sci., 2026, 17, 12249–12278 | 12271Fig. 39 A compartmentalized nanostructure used to regulate bioenergetic levels. Encapsulated glucose dehydrogenase (GDH), urease andnicotinamide adenine dinucleotide drive an oscillatory proton gradient, which creates an oscillatory cycle of ATP synthesis and decompositioncontrolling bioenergetic levels in opposing directions. Reprinted with permission from ref. 70, Copyright 2024 Wiley-VCH.Chemical Science Reviewto integrate these biomolecular machines, in addition tonanoarchitectonics approaches for their manipulation, is of theutmost importance.Fig. 40 Switchable, non-equilibrium, hydrodynamic assembly andphase separation in a suspension of acoustically driven, chiral micro-spinners. The 3D chirality of the spinners drives self-assembly inparallel planes, forming a 3D hierarchical system. The twisted 3Dstructure introduces system-wide chirality. Reprinted with permissionfrom ref. 71, Copyright 2023 American Chemical Society.Collective behaviour of microrobotsIn addition to molecular and biomolecular machines, there arealso nanorobots and microrobots: nano- and microscale func-tional materials that behave like machines. Distinct frommolecular machines, they are designed with and synthesizedfrom nanomaterials and micromaterials rather than individualmolecules or biomolecules. Although they are larger thanmolecular machines, their collective behaviour is no lessinteresting or functional. In this section, we examine severalexamples of studies featuring collective behaviour ofmicrorobots.Controlling the interactions of large-scale synthetic particleswarms could lead to similar macroscopic robotic systemspossessing microscopic complexity. Rotation-induced self-assembly has been reported in biological systems. Kagan,Mallouk and co-workers reported switchable, non-equilibrium,hydrodynamic assembly and phase separation in a suspensionof acoustically driven, chiral micro-spinners (Fig. 40).72 Semi-quantitative modelling suggests that in this system, the 3Dcomplex spinners interact via viscous forces and weak inertialstreaming. The 3D chirality of the spinners drives self-assemblyin parallel planes, forming a 3D hierarchical system. Thistwisted 3D structure effectively introduces system-widechirality. Such 3D microspinners may provide a framework forengineering more complex systems at the particle level, withanticipated contributions in physical science. Further efforttowards incorporating new layers and complex particle types isanticipated.Controlled release and precise enrichment of microrobotswarms have the potential to signicantly enhance detectionspeeds and selectivity in biosensing and chemical analysis. Luet al. demonstrated an efficient and versatile strategy fordispersing and aggregating individual micromotors usinga needle-like hybrid sonoelectrode (Fig. 41).72 This strategysignicantly accelerates mass transfer and enhances the signalintensity. In their system, hydrogen bubbles are generated at12272 | Chem. Sci., 2026, 17, 12249–12278the tip of a charged electrode and vibrated by an acoustic eld tocreate strong vortices that disperse the micromotors sponta-neously. By removing the attached bubble, the sonoelectrodeacts as a solid-needle isolator. This generates acousticstreaming within the actuation reservoir using high-frequencyultrasound, enabling the large-scale collection of micro-motors. This system has the potential to control micromotorswarming behaviour with versatility and speed, facilitating thedevelopment of intelligent microrobots with active enrichment© 2026 The Author(s). Published by the Royal Society of ChemistryFig. 41 Dispersing and aggregating individual micromotors using a needle-like hybrid sonoelectrode. Hydrogen bubbles are generated at the tipof a charged electrode and vibrated by an acoustic field to create strong vortices that disperse the micromotors spontaneously. By removing thebubbles, the sonoelectrode acts as a solid-needle isolator that drives micromotor aggregation. Reprinted with permission from ref. 72, Copyright2021 Wiley-VCH.Review Chemical Sciencecapabilities compatible with next-generation, highly sensitive,portable detection microsystems. This strategy could be appliedin next-generation wearable microsystems for active, high-precision biochemical analysis and ultratrace-level detection.Magnetic nanorobot swarms can mimic collective behaviourfound in nature. These swarms can be exibly controlled withprogrammable magnetic elds, boasting great potential fora variety of applications. Chen et al. reported a novel approachto the rapid and scalable fabrication of laser-induced graphene(LIG)-based Fe3O4 nanorobot swarms using a one-step UV laserprocessing technique (Fig. 42).73 These swarms can formvarious reversible morphologies, including vortices and strips,in response to magnetic elds. Furthermore, these morphol-ogies can interconvert, demonstrating high controllability andexibility. The drug loading and release performance utilizingthese nanorobot swarms improved by approximately 50-foldcompared to individual carriers. Furthermore, drug-loadedswarms can pass smoothly through zigzag channels of varyingwidths while retaining 96% of the initial drug payload. Loading,release, and targeting of doxorubicin (DOX) using these nano-particle swarms under magnetic eld control has beendemonstrated. This study sheds light on the processing ofnanorobot swarms and their application as high-performance,targeted drug delivery systems.Many high demand and high impact applications requiremobile microrobots to form cohesive swarms in unboundedFig. 42 Laser-induced graphene (LIG)-based Fe3O4 nanorobot swarmsresponse to magnetic fields. Drug-loaded swarms can pass smoothly throdrug loading for targeted release. Reprinted with permission from ref. 73© 2026 The Author(s). Published by the Royal Society of Chemistryconditions. Sitti and his team discovered that balancingmagnetic dipole attractions and multipole repulsions enablesself-assembled particle-chain microrobots to self-organize intocohesive clusters (Fig. 43).74 The microrobots themselves wereformed through dynamic self-organization of paramagneticparticles into anisotropic linear chains. At a specic openingangle of the processing magnetic eld, magnetic interactionsbetween the chains induce slowly decaying dipole attractionsand rapidly decaying multipole repulsions. These opposingeffects result in an equilibrium distance between pairs wherethe sum of the dipole and multipole forces is zero. Undercohesive interactions, the chains self-organize into clusters byaligning at an equilibrium distance from neighbouring chains.The scalability of cohesive interactions enables larger groups toform, and their internal spatiotemporal organization can tran-sition from a solid-like state to a liquid-like state as the clusterincreases in size. Additionally, cluster velocity was found toincrease with cluster size due to collective hydrodynamiceffects. This work achieved operation of microrobots as local-ized swarms, and has potential to inspire the design ofadvanced ensemble systems for application in biomedicine,precisionmanipulation andmanufacturing, and environmentalsensing and remediation.Many biological systems, such as birds and sh, exhibitcollective behaviours such as schooling. Analogous behaviourhas been reported in active colloidal particles, which coordinateform various reversible morphologies, including vortices and strips inugh zigzag channels of varying widths while retaining 96% of the initial, Copyright 2024 American Chemical Society.Chem. Sci., 2026, 17, 12249–12278 | 12273Fig. 43 Paramagnetic particles dynamically self-organize of pinto anisotropic linear chains. These linear chains act as microrobots that furtherself-organize into clusters when they spontaneously align under inducedmagneticmoments. As the clusters increase in size, they transition froma solid-like state to a liquid-like state. Additionally, cluster velocity also increases with size due to collective hydrodynamic effects. Reproducedunder the terms of the CC-BY license from ref. 74, 2020 Royal Society of Chemistry.Fig. 44 Magnetically driven swarm of living bacterial microrobots forthe purification of aquatic microplastics and nanoplastics. Themicrorobots can propel themselves via flagellar movement. Addi-tionally, they can be collectively steered with a rotating magnetic field.The multimodal operation of these microrobots which replicates 3Dswarming navigation, not unlike a school of fish. This allows activecapture of micro- and nanoplastics in a biomechanical solution to themicroplastics pollution crisis. Reproduced under terms of the CC-BYlicense from ref. 76, 2025 American Chemical Society.Chemical Science Reviewthe movement of subsidiary particles that make up micro-robots. Liu and Dijkstra used Brownian dynamics simulationsto study the 3D collective behaviour of intelligent active Brow-nian spheres, rods and nematodes.75 This study used computersimulations to examine intelligent active Brownian particleswith visual perception and 3D velocity alignment. These parti-cles exhibit a tendency to move towards their centre of masswhile velocity alignment promotes synchronization withneighbouring particles. Reducing the size of the simulation boxrevealed new structures, such as band-like clusters and dense“baitballs”. Rod-like particles formed band-like, worm-like,radial and spiral structures. Worm-like particles exhibitedband-like, streamlined, micellar and entangled structures.Many of these patterns resemble collective behaviours observedin nature, such as ant milling, sh baitballs and worm-likeclusters. Advances in synthesis could lead to the creation ofnanorobots with similar functions, which could in turn providevaluable insights into multicellular systems by way of studyingactive substances.As mentioned above, the collective behaviour of microrobotsexhibits similarities to those seen in biological systems. Someresearchers have built on this concept by incorporating livingorganisms into microrobots. For example, Pumera and co-workers proposed a magnetically driven swarm of living bacte-rial microrobots for the purication of aquatic microplasticsand nanoplastics (Fig. 44).76 The combination of magneticallyguided navigation and autonomous propulsion enables themultimodal operation of a swarm of magnetotactic-bacteria-based living microrobots. A rotating magnetic eld induces3D swarming navigation similar to that of a school of sh,actively capturing micro- and nanoplastics. These are then12274 | Chem. Sci., 2026, 17, 12249–12278recovered from contaminated water by magnetic separation.Actuation of these microrobots combines autonomous self-propulsion via agellar movement with precise, untethered© 2026 The Author(s). Published by the Royal Society of ChemistryReview Chemical Sciencenavigation controlled via the magnetic eld. This enablesmultimodal steering, such as directional propulsion or rotarycircular motion. These magnetotactic-bacteria-based livingmicrorobots exhibiting swarm behaviour present a biomechan-ical solution that may nd use in the impending microplasticspollution crisis.Although microrobots are larger than molecular machines,they share the same reliance on collective structural organiza-tion. Their behaviour is not unlike a swarm of living organisms,and their use in practical applications such as the cleanup ofmicroplastics shows promise. Their advantage over molecularmachines is ease of observation and simulation. The collectivebehaviour of microrobots is very important, as the collectiveaction of many units sum ups to larger-scale function. While theeffects of microscopic thermal uctuations and Brownianmotion on molecular machines and microrobots differ, micro-robot behaviours could nevertheless yield valuable insights intothe collective behaviour of molecular machines.Future perspectiveThis review has explored collective behaviours in molecularmachines and microrobots, nding trends in collective behav-iours and their associated material systems and environments.We have placed emphasis on the paradigm shi from solitary tocollective behaviour, examining how this is reected in func-tionally organized materials. Applying the concept of nano-architectonics to molecular machines and microrobots couldfacilitate the deliberate design of functional material systems atthe nanoscale.We identied several distinct collective behaviour patterns,the most notable of which are: (i) multiple molecular machinesoperating independently, with the sum of unique molecularfunctions producing a signicant macroscopic output; (ii)conversely, collective structures can also drive individualmolecular machines through macroscopic actions and forces;(iii) more advanced collective structures in which molecularmachines work synchronously like force-transducing gears; and(iv) even without physical, gear-like force transduction interac-tions, systems of diverse molecular machines (includingbiomolecular machines) with linked outputs can produce moreadvanced mechanical and functional system outputs.The many examples presented in this review demonstratethat the collective behaviours of molecular machines arestrongly correlated with their environment. This can besummarized as follows: (i) regularly ordered porous materials,such as metal–organic frameworks (MOFs) and covalent organicframeworks (COFs), provide nanospaces in which molecularmachines can move freely. The collective action of molecularmachines within MOFs and COFs is an attractive strategy forconverting molecular function into practical output. (ii) Crys-tals, despite not providing nanospaces like MOFs do, insteadprovide ordered structures in which molecular machines canperform collective behaviours in a controlled manner. Theability to construct materials with integrated molecular gearstructures provides a methodology for coupling motion at themolecular level with macroscopic material properties.© 2026 The Author(s). Published by the Royal Society of ChemistryFurthermore, the shape and motion of molecular machines canbe directly observed on solid surfaces, enabling the design ofsophisticated collective behaviours involving molecular gearsmeshing and interacting with molecular rotors. The operationalbehaviour of molecular machines can also be studied at thequantum level through molecular observations using STM andtheoretical calculations. (iii) At the air–water interface, couplingof macroscopic mechanical motion to molecular motion can beachieved. Integrating molecular machines at an interfaceenables them to be driven by macroscopic mechanical stimuliand allows the function of molecular receptors to be optimized.Using liquid interfaces such as the air–water interface isa methodology with great potential for opening up new scien-tic elds.Expanding the scope from relatively small, organicallysynthesized molecular machines to biomolecular machinesmade from large biological molecules or even larger micro-robots, different collective characteristics are observed. Onemajor advantage of systems in which multiple biomolecularmachines work together is their suitability for creating functionows integrating the effects of different machines in a singlesystem. Biomolecular machines have innately sophisticatedfunctions, and their organizational manipulation can yieldlarger functions greater than the sum of their parts. This is notunlike collective behaviours in living organisms, and articial,deliberate design is anticipated to give form to machinescomparable to, or even surpassing those seen in living organ-isms. These characteristics have practical importance, as theirapplication to solving real world problems such as the recoveryof microplastics has been demonstrated.Molecular machines are at the pinnacle of nanoscience,having realized nano- and microscopic objects that functionlike machines. They have even won a Nobel Prize. However,more technological advancements are necessary before thesematerials nd widespread practical use. A crucial step is toassemble individual molecular machines into objects that canfunction collectively, with the aid of nanoarchitectonics meth-odologies. This review found correlations between molecularmachines' properties and their environment and morphology,identifying tendencies for certain collective forms to exhibitcorrespondent functions. Interfaces are particularly enablingfor organizational manipulation of molecular machines toresult in useful and impactful functions. To advance the prac-tical application of these sciences and technologies, holisticcombination of conventionally distinct research elds isnecessary to inspire designs transcending the systemsdescribed in this work. In particular, the deliberate design andsynthesis of functional systems combining and coordinatingthe functions of multiple molecular machine elements isessential. Designing such complex systems requires synthesisinformed by accumulated experience from countless materialsscience experiments and vast amounts of data. As such, theintervention of articial intelligence (AI), and moreover AI-based nanoarchitectonics, has been in demand.77 Buildingcomplex assemblies by manipulating molecular machinesusing this approach is anticipated to accelerate the fruition ofhighly functional systems that match, or even exceed theChem. Sci., 2026, 17, 12249–12278 | 12275Chemical Science Reviewstrategies used by the living organisms that inspired them. Thisis an ultimate goal for functional materials chemistry.Author contributionsConceptualisation K. A. and J. S.; collecting literature K.A., W. L. and J. S.; writing – original dra, review and editing K.A., W. L. and J. S.; supervision K. A.; funding acquisition K. A.Conflicts of interestThere are no conicts to declare.Data availabilityNo primary research results, soware or code have beenincluded, and no new data were generated or analysed as part ofthis review.AcknowledgementsThis study was partially supported by Japan Society for thePromotion of Science KAKENHI (Grant No. JP23H05459 andJP25H00898). K. A. would like to thank Prof. Mingoo Jin inHokkaido University for important literature information andscientic advice. We all thank Dr Xuechen Shen for professionalEnglish correction.Notes and references1 (a) J. Li and B. Chen, Chem. 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Published by the Royal Society of Chemistry Nanoarchitectonics of molecular machines, biomolecular machines, and microrobots in their collective behaviour Nanoarchitectonics of molecular machines, biomolecular machines, and microrobots in their collective behaviour Nanoarchitectonics of molecular machines, biomolecular machines, and microrobots in their collective behaviour Nanoarchitectonics of molecular machines, biomolecular machines, and microrobots in their collective behaviour Nanoarchitectonics of molecular machines, biomolecular machines, and microrobots in their collective behaviour Nanoarchitectonics of molecular machines, biomolecular machines, and microrobots in their collective behaviour Nanoarchitectonics of molecular machines, biomolecular machines, and microrobots in their collective behaviour Nanoarchitectonics of molecular machines, biomolecular machines, and microrobots in their collective behaviour Nanoarchitectonics of molecular machines, biomolecular machines, and microrobots in their collective behaviour Nanoarchitectonics of molecular machines, biomolecular machines, and microrobots in their collective behaviour Nanoarchitectonics of molecular machines, biomolecular machines, and microrobots in their collective behaviour Nanoarchitectonics of molecular machines, biomolecular machines, and microrobots in their collective behaviour Nanoarchitectonics of molecular machines, biomolecular machines, and microrobots in their collective behaviour Nanoarchitectonics of molecular machines, biomolecular machines, and microrobots in their collective behaviour