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[Katsuhiko Ariga](https://orcid.org/0000-0002-2445-2955)

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[Fascinating Frontier, Nanoarchitectonics, as Method for Everything in Materials Science](https://mdr.nims.go.jp/datasets/4a70d462-d4c7-4f25-83f7-e3c6d31e3800)

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Fascinating Frontier, Nanoarchitectonics, as Method for Everything in Materials ScienceAcademic Editor: Werner BlauReceived: 20 October 2025Revised: 11 November 2025Accepted: 13 November 2025Published: 15 November 2025Citation: Ariga, K. FascinatingFrontier, Nanoarchitectonics, asMethod for Everything in MaterialsScience. Materials 2025, 18, 5196.https://doi.org/10.3390/ma18225196Copyright: © 2025 by the author.Licensee MDPI, Basel, Switzerland.This article is an open access articledistributed under the terms andconditions of the Creative CommonsAttribution (CC BY) license(https://creativecommons.org/licenses/by/4.0/).ReviewFascinating Frontier, Nanoarchitectonics, as Method forEverything in Materials ScienceKatsuhiko Ariga 1,21 Research Center for Materials Nanoarchitectonics (MANA), National Institute for Materials Science (NIMS),1-1 Namiki, Tsukuba 305-0044, Japan; ariga.katsuhiko@nims.go.jp2 Graduate School of Frontier Sciences, The University of Tokyo, 5-1-5 Kashiwanoha, Kashiwa 277-8561, JapanAbstractMethodological fusion of materials chemistry, which enables us to create materials, withnanotechnology, which enables us to control nanostructures, could enable us to createadvanced functional materials with well controlled nanostructures. Positioned as a post-nanotechnology concept, nanoarchitectonics will enable this purpose. This review paperhighlights the broad scope of applications of the new concept of nanoarchitectonics, se-lecting and discussing recent papers that contain the term ‘nanoarchitectonics’ in theirtitles. Topics include controls of dopant atoms in solid electrolytes, transforming theframework of carbon materials, single-atom catalysts, nanorobots and microrobots, func-tional nanoparticles, nanotubular materials, 2D-organic nanosheets and MXene nanosheets,nanosheet assemblies, nitrogen-doped carbon, nanoporous and mesoporous materials,nanozymes, polymeric materials, covalent organic frameworks, vesicle structures fromsynthetic polymers, chirality- and topology-controlled structures, chiral helices, Langmuirmonolayers, LB films, LbL assembly, nanocellulose, DNA, peptides bacterial cell compo-nents, biomimetic nanoparticles, lipid membranes of protocells, organization of livingcells, and the encapsulation of living cells with exogenous substances. Not limited to theseexamples selected in this review article, the concept of nanoarchitectonics is applicableto diverse materials systems. Nanoarchitectonics represents a conceptual framework forcreating materials at all levels and can be likened to a method for everything in materialsscience. Developing technology that can universally create materials with unexpectedfunctions could represent the final frontier of materials science. Nanoarchitectonics willplay a significant part in achieving this final frontier in materials science.Keywords: atomic and molecular level structure; biological material; living cell;nanoarchitectonics; nanomaterial; nanostructured functional material; polymeric material;supramolecular chemistry1. IntroductionAdvances in information technology (IT) are transforming our lifestyles. Further-more, remarkable advances in artificial intelligence (AI) are bringing about further socialchange. Although significant progress has been made in cyberspace, this is based onthe development of functional materials in the real world. Today’s society faces manychallenges. Furthermore, improvements to everyday life are constantly being pursued.Addressing these challenges requires the development of functional materials that cansolve these issues. The active development of functional materials for a variety of appli-cations is currently underway. Energy-related technologies, such as fuel cells [1–6], solarMaterials 2025, 18, 5196 https://doi.org/10.3390/ma18225196https://doi.org/10.3390/ma18225196https://doi.org/10.3390/ma18225196https://creativecommons.org/licenses/by/4.0/https://creativecommons.org/licenses/by/4.0/https://www.mdpi.com/journal/materialshttps://www.mdpi.comhttps://orcid.org/0000-0002-2445-2955https://doi.org/10.3390/ma18225196https://www.mdpi.com/article/10.3390/ma18225196?type=check_update&version=2Materials 2025, 18, 5196 2 of 36cells [7–12] and other energy generation technologies [13–17], various batteries [18–22] andsupercapacitors [23–28], are exploring useful materials and how to structure them. Thisresearch trend is also prevalent in ecology and the environment, including the detectionof specific substances [29–34], the removal of pollutants [35–39] and microplastics [40–45],achieving carbon neutrality [46–50], and the effective use of biomass [51–56]. In biomedicalfields such as drug delivery [57–62], biosensing [63–67], virus prevention [68–70], cancertreatment [71–73] and various medical technologies [74–80], the development of functionalmaterials—not just biochemical technologies—holds the key. Furthermore, developingsemiconductor materials [81–84] and controlling their functions [85–90] are important fordevices and sensors that support information technology. While the development of suchfunctional materials appears to be progressing in a specific way at first glance, there is aconsistent flow. It is necessary to develop materials individually to meet various targetsand demands. However, it is even more important to take a step back and understandthe broader trends in scientific and technological development. Such an understandingenables diverse developments to be interconnected, leading to more rational scientific andtechnological progress. So, where are materials science and technology headed? Ratherthan focusing on the development of methods or techniques for creating specific products,this review discusses a unified, comprehensive concept of materials science. To this end,this review provides an overview of developments in materials science and nanotechnologyto date, introducing the concept of nanoarchitectonics as a successor to these fields. Ratherthan considering this concept systematically, this review demonstrates its application inmany fields through showing divers applicable targets. This illustrates the broad impactthat the concept can have. The purpose of this review is to explore the future of materialsscience comprehensively, rather than presenting anything specific.In the early stages, humanity sought to improve life’s conveniences by procuringuseful materials from nature. Through experience, they also learned the techniques toprocess these materials and modify them into alloys and other substances. However,this trend was fundamentally changed by advances in materials science, particularly inthe 20th century. Instead of being limited to using raw materials obtained from nature,it became possible to create new materials through systematic academic research. Thistrend continues to this day. While efforts are being made to analyze structures [91–94]and understand phenomena [95–101] in fields such as physics, physical chemistry andbiology, advances in materials-related chemistry that can create new materials have hada significant impact. The creation, understanding and utilization of new functional ma-terials through organic chemistry [102–106], inorganic chemistry [107–113], coordinationchemistry [114–118], polymer chemistry [119–126], other materials chemistry [127–132] andbiochemistry [133–139] continues to this day. Breakthroughs in materials-related chemistryhave been instrumental in advancing humanity.Throughout this ongoing development, humanity has realized a very importantfact. While the properties and functions of a material are important, its structure alsoplays a vital role. Even the same material can have dramatically improved or entirelynew functions when its size and internal structure differ. Controlling its structure atthe nanoscale is particularly effective. Nanostructures offer many advantages. Whenmaterials are manipulated at an extremely small scale, phenomena such as quantumeffects [140–144] emerge. Nanostructured materials have a significantly larger interfacialarea per unit volume, which enhances their catalytic functions [145,146]. Organizingfunctional units at the nanoscale enables efficient energy and electron transfer [147,148].In other words, developing materials with more advanced functions requires controllingthe material’s nanostructure as well as developing the materials themselves. The adventof nanotechnology has clearly initiated this research trend. Nanotechnology continuesMaterials 2025, 18, 5196 3 of 36to evolve actively today. It is now possible to observe [149–152], manipulate [153–156]and study phenomena [157–165] at the atomic, molecular, and nanoscopic levels. Thesetechniques have become indispensable for understanding materials and phenomena. Itcould be argued that the development of nanotechnology represents a second breakthroughin the development of functional materials.The next step will require the development of an integrated concept. This could repre-sent a significant milestone in the development of functional materials. In other words, weneed to combine materials chemistry, which enables us to create materials, with nanotech-nology, which enables us to control nanostructures. Positioned as a post-nanotechnologyconcept, nanoarchitectonics will enable this purpose (Figure 1) [166]. Just as Richard Feyn-man pioneered nanotechnology in the mid-20th century [167,168], Masakazu Aono pro-posed nanoarchitectonics during the transition from the 20th to the 21st century [169,170].Nanoarchitectonics integrates nanotechnology and materials chemistry to build functionalmaterial systems from basic elements such as atoms, molecules and nanomaterials [171].Nanoarchitectonics is not an entirely new concept. Rather, it seeks to integrate existingconcepts and create a stream of clear breakthroughs. Methods of assembling atoms andmolecules to create functional structures have been realized through self-assembly insupramolecular chemistry and related fields such as molecular/materials assembly sci-ence [172–176], metal–organic frameworks (MOFs) [177–183] in coordination chemistry,and covalent organic frameworks (COFs) [184–188], which have been cleverly developedfrom polymer chemistry. Mesoporous and related materials [189–193] have also been cre-ated by materials chemistry using molecular assemblies as templates. In interface science,the construction of functional thin films from molecules and materials has been widelydemonstrated using methods such as self-assembled monolayers (SAMs) [194–199], theLangmuir–Blodgett (LB) method [200–204] and layer-by-layer (LbL) assembly [205–209].However, this concept has developed rather independently and has not become a unifieddriving force in research. The importance of creating an integrated concept, even if it is notentirely novel, is evident from the success of nanotechnology. Although there was a needfor research to elucidate nano-level phenomena, it was nanotechnology that became a sym-bolic unifying concept, leading to the creation of a major research trend. Nanoarchitectonicsis now taking on this role. Figure 1. History and outline of the nanoarchitectonics concept.Materials 2025, 18, 5196 4 of 36Nanoarchitectonics involves building functional materials using existing knowledgeand technologies. This process involves creating materials that incorporate a varietyof technological elements. Building functional material systems from atoms, molecules,and nanomaterials can incorporate a variety of technologies and sciences. These ma-terials can be created by selecting and combining atomic and molecular manipulation,chemical transformations (including organic synthesis), physical transformations, self-assembly/self-organization, orientation induced by external forces or fields, nanofabrica-tion/microfabrication and biochemical processes [210]. Unlike conventional supramolec-ular methods such as self-assembly, MOF and COF, the nanoarchitectonics processes aresupposed to comprehensively integrate several methods together even including physi-cal fabrication and biological treatments. These integrated material fabrication methodsalso offer advantages in terms of structural fabrication. Compared to single processes orprocesses based on a single equilibrium, combining multiple processes offers significant ad-vantages when it comes to building asymmetric and hierarchical structures [211]. However,nanoscale interactions can sometimes involve uncertainty, including contributions fromthermal fluctuations and quantum effects [212]. The inputs added to functional materialsdo not necessarily equate to the sum of their components as they interfere with each other.Therefore, rather than being additive, the effect is that of a harmonized whole [213]. This isvery similar to the functional systems of living organisms, in which multiple functionalunits link together and work collaboratively within thermal fluctuations. This is a com-mon characteristic of nanoarchitectonics. Conversely, one could argue that the ultimategoal of nanoarchitectonics is to build highly functional systems similar to those found inliving organisms [214].The principles and characteristics of nanoarchitectonics are general and universal,and are independent of the materials used, their functions, and their applications. In re-cent years, the number of papers claiming to be in this field has increased. The rangeof papers featuring the term ‘nanoarchitectonics’ in their titles is diverse. Many fo-cus on basic science, such as the study of chemical materials [215–219] and structuralcontrol [220–223], the exploration of physical phenomena [224,225], and fundamentalbiochemical approaches [226–230]. However, nanoarchitectonics is also widely used inapplication-oriented fields, including solar cells [231–234], fuel cells [235–239], batter-ies [240–243], supercapacitors [244–249] and other energy applications [250–254], environ-mental issues [255–258], catalysis [259–264], devices [265–269], sensors [270–273], biosen-sors [274–277], drug delivery [278–282] and biomedical applications [283–288]. As allmaterials are essentially composed of atoms and molecules, the nanoarchitectonics method-ology, which is built from these components, may be applicable to all materials. If theultimate goal of physics is to establish a theory of everything [289], nanoarchitectonicscould be considered a method for everything in materials science [290,291]. Nanoarchitec-tonics is also the final frontier in the quest to assemble highly functional systems akin tothose found in living organisms. The challenge of nanoarchitectonics is to achieve, withinour own lifetimes, a feat equivalent to the creation of highly functional systems from atomsand molecules, which evolution in nature has taken billions of years to achieve.To this end, this review paper will introduce the concept of nanoarchitectonics byhighlighting recent papers that include the term in their title. Finally, future directions willbe discussed in reference to these examples. Next, this paper will discuss the potential ofnanoarchitectonics as a method for a wide range of applications. Its perspective sectionwill also consider what is required for nanoarchitectonics to become the ultimate frontier inthe development of functional materials.Materials 2025, 18, 5196 5 of 362. Research Target in Nanoarchitectonics from Atom to Living CellTo demonstrate the widespread use of the concept of nanoarchitectonics, this sectionpresents a number of examples of research papers. To illustrate its deep involvementin research, only papers containing the term ‘nanoarchitectonics’ in the title have beenselected. Many of the examples are from recent papers, showing that nanoarchitectonics isused in popular research fields. Furthermore, to demonstrate the wide range of researchcontent targeted, the papers have been selected to show divergence rather than systematicorganization. Because these examples have various functions with certain integration, theexamples are basically represented in the order of system sizes from atoms and moleculesto materials and living systems. One strict selection criterion is that these research exampleshave the term of nanoarchitectonics in their paper title. Because of rapid growth of nanoar-chitectonics research in these days, the most of them are selected from those published inthese few years.2.1. Nanoarchitectonics for Dopant AtomIn their paper, ‘Nanoarchitectonics for controlling the number of dopant atoms in solidelectrolyte nanodots’, Hasegawa et al. reported a method for controlling the number ofdopant atoms in solid electrolytes [292]. This represents a nanoarchitectonics strategy forachieving discrete electrical properties. Controlling the movement of electrons and holes isa key challenge in today’s highly information-driven society. The ultimate technology insolid-state nanoionics, aimed at applications in energy storage, sensing and brain-basedinformation processing, is the ability to control material properties at the atomic scale. Theproposed study uses α-Ag2S nanodots containing non-stoichiometric excesses of Ag+ ionsand electrons as a model system. The dopant can be controlled and manipulated in discretesteps by changing the electrochemical potential. In thermodynamic equilibrium, the Gibbsfree energy of solid electrolyte materials can be minimized through the formation of pointdefects, i.e., Frenkel or Schottky equilibrium. The number of defects increases when oneof the components is non-stoichiometric. This significantly affects the electronic and/orionic conductivity of the material. In particular, as approaching to the nanoscale, theequilibrium defect concentration can increase by orders of magnitude due to the increasedentropy of the system. By limiting the size of nanodots, the number of nonstoichiometricdefects that function as dopants and undergo electrochemical transformation can be tai-lored. This approach proposed a strategy for controlling the number of dopant atoms inα-Ag2+δS nanodot solid electrolytes on platinized silicon wafer substrates by adjusting theelectrochemical potential. Limiting the number of non-stoichiometric dopants increasesthe distance between adjacent electrochemical potential levels, enabling the precipitationof atoms. This approach is an attractive paradigm in nanoarchitectonics for developingnanodevices based on single-ion/single-atom transfer.2.2. Nanoarchitectonics for Pentagon Defect in CarbonResearch into nanoarchitectonics, which involves manipulating the carbon atom frame-work in carbon materials at the atomic level, has also been reported. Chen et al. recentlyreported a method for controlling the oxygen reduction reaction (ORR) by manipulatingpentagon structures in carbon materials [293]. In their review paper, ‘Nanoarchitectonics forpentagon defects in carbon: properties and catalytic role in oxygen reduction reaction’, Chenet al. provide a comprehensive summary of the formation mechanism, characterization,spin, oxygen adsorption and ORR catalytic activity of carbon catalysts containing pentagondefects [294]. Carbon materials have attracted considerable attention as a sustainable andeconomical alternative to noble metal catalysts. In recent years, it has been reported thatintroducing pentagon structures into graphitic carbon promotes ORR catalytic activity. AsMaterials 2025, 18, 5196 6 of 36illustrated in Figure 2, this review explores the formation mechanism of pentagon defectsin carbon materials, from high-temperature annealing to bottom-up synthesis strategies.Notably, carbon catalysts containing pentagons exhibit high catalytic activity even underacidic conditions and often outperform N-doped carbon catalysts. These catalysts arehighly durable and approach the ORR performance of Pt-based catalysts. This high activityis attributed to the unique electronic structure induced by the pentagonal defects whichlead to spin formation. Pentagonal structures have been introduced into carbon frame-works using various nanoarchitectonics methods, including high-temperature treatment,bottom-up synthesis and selective dopant removal. Furthermore, considerable attentionhas also been given to the synergistic effect of heteroatom dopants, such as nitrogen andsulphur, with pentagonal defects. Figure 2. Summary of studies of pentagon-containing carbon catalysts for oxygen reduction reaction(ORR). Reproduced under terms of the CC-BY license [294]. Copyright 2025 Wiley-VCH.2.3. Single-Atom Nanoarchitectonics for Oxygen Evolution ReactionThe design of single-atom catalysts is also being explored in nanoarchitectonics. Oneof the key targets for catalysis is the development of electro-catalysts for the oxygenevolution reaction (OER), which are essential for producing green hydrogen through waterelectrolysis but also present a significant research challenge. In their paper, ‘Ru single-atom nanoarchitectonics on Co-based conducting metal–organic frameworks for enhancedoxygen evolution reaction’, Du, Xu and coworkers prepared ruthenium (Ru) single-atom-decorated Co-HHTP (HHTP = 2,3,6,7,10,11-hexahydroxytriphenylene) (Ru@Co-HHTP)using solvothermal and ion-exchange methods (Figure 3) [295]. First, Co(OH)2 was grownon a substrate using a solvothermal method and then converted to Co-HHTP by addingHHTP during the solvothermal process. Furthermore, a single Ru atom was immobilizedon the Co-HHTP using an ion-exchange method. This study aims to demonstrate thatintroducing atomically dispersed Ru into Co-HHTP increases the electrochemically activearea, improves charge transfer capability and optimizes the electronic structure of Co-HHTP. Systematic experiments suggest that atomically dispersed Ru can optimize theelectronic structure and electronic conductivity of Co-HHTP, resulting in low overpotential,a small Tafel slope, a large electrochemically active surface area, an excellent charge transfercapability and a strong electronic interaction between Co and Ru. Consequently, excellentOER performance was demonstrated. Furthermore, this is expected to greatly acceleratethe development of alkaline water splitting for practical applications.Materials 2025, 18, 5196 7 of 36 Figure 3. Introduction of atomically dispersed Ru into Co-HHTP (HHTP = 2,3,6,7,10,11-hexahydroxytriphenylene) for excellent oxygen evolution reaction (OER) performance. Reprintedwith permission from [295]. Copyright 2024 American Chemical Society.2.4. Single-Atom Nanoarchitectonics for RoboticsThe development of nanoarchitectonics, which involves creating objects that functionlike nanorobots and microrobots, is also underway. The ultimate goal of this field ofresearch is to construct highly precise, functional, dynamic systems originating at theatomic and molecular level. In such robotic structures, single-atom catalysts act as activecomponents that power the robots. In their review paper, ‘Single-atom nanoarchitectonicsfor robotics and other functions’, Jancik-Prochazkova et al. discuss functional systemsimplemented with single-atom catalysts as active elements in the field of nano/micro-robotics (Figure 4) [296]. Single-atom-modified nano/microrobots are dynamic systemsthat utilize the catalytic activity of single atoms and can enhance propulsion or providecatalytic functionality. The review paper covers three key topics: research trends in single-atom catalysts, single-atom-modified nano/microrobots and additional applications ofsingle-atom nanoarchitectonics. It also considers the future development and direction ofsingle-atom-modified nano/microrobots. It is particularly expected that the next generationof intelligent single-atom-modified nano/micro-robots will be developed using artificialintelligence (AI). Figure 4. Basic concept for single-atom nanoarchitectonics for robotics and other functions. Repro-duced under terms of the CC-BY license [296]. Copyright 2025 American Chemical Society.Materials 2025, 18, 5196 8 of 362.5. Nanoarchitectonics of NanoparticleFunctional nanoparticles and related nanostructures are important targets in thefield of nanoarchitectonics. In their paper, ‘Nanoarchitectonics of CdFe2O4 nanoparticleswith different morphologies synthesized using a thermal decomposition approach andstudies of their peroxidase-like activity’, Gangwar and Jeevanandam reported that CdFe2O4nanoparticles with different morphologies can be synthesized using a simple thermaldecomposition method with Cd–Fe glycolate as a precursor [297]. Varying the reactionconditions resulted in CdFe2O4 nanoparticles with various morphologies, such as flake,raspberry and hexagonal (Figure 5). Nucleation and growth are key factors affecting themorphology of Cd–Fe glycolate. The synthesis temperature influences these factors, andnanoparticles of various shapes are formed through kinetic control and surface energyreduction. Furthermore, CdFe2O4 nanoparticles exhibit morphology-dependent magneticproperties. Furthermore, CdFe2O4 nanoparticles exhibit peroxidase-like activity in thepresence of hydrogen peroxide. The catalytic activity of CdFe2O4 nanoparticles is affectedby their morphology, particle size, surface area and Fe3+ ion concentration. Their catalyticactivity is superior to that of the natural enzyme horseradish peroxidase (HRP). CdFe2O4nanoparticles may be useful in applications such as magnetic devices, catalysis and sensing. Figure 5. Nanoarchitectonics of CdFe2O4 nanoparticles with different through varying the reactionconditions where nucleation and growth are key factors affecting the morphology of Cd–Fe glycolate.Reprinted with permission from [297]. Copyright 2024 Royal Society of Chemistry.2.6. Tubular NanoarchitectonicsResearch on nanoarchitectonics of tubular materials has also been reported. Vanadiumsulfide has attracted attention as a potential anode material for sodium-ion batteries.However, its electrochemical performance is limited by poor structural stability duringcharge–discharge processes and a slow ion diffusion rate. In a paper titled ‘Tubularnanoarchitectonics of titania@vanadium–sulfide/bismuth–sulfide composite for effectivesodium-ion storage’, Huang et al. developed a material in which VS4/Bi2S3 nanorods wereimmobilized on the surface of titania nanotubes (Figure 6) [298]. Cellulose-derived titaniananotubes were employed as a structural scaffold for synthesizing this material usingsol–gel and hydrothermal methods. A metal sulfide-based double-tubular nanostructure(TiO2@VS4/Bi2S3 composite) was then constructed on this scaffold. This composite consistsof VS4/Bi2S3 nanorods grown on the surface of the titania tubes, forming a heterogeneousinterface with abundant voids and mesopores. The composite’s excellent sodium storageMaterials 2025, 18, 5196 9 of 36properties are attributed to its abundant phase interfaces and cross-linked tubular structure.The cross-linked TiO2@VS4/Bi2S3 nanotube composite effectively improves the kinetics ofcharge transfer and sodium ion transport and alleviates the problems of volume expansionand voltage drop. Given the common challenges involved, this study may offer valuableinsights into designing heterogeneous nanocomposites with abundant phase interfaces. Figure 6. Tubular nanoarchitectonics of titania@vanadium-sulfide/bismuth-sulfide composite foreffective sodium-ion storage, in which cellulose-derived titania nanotubes were employed as astructural scaffold for synthesizing this material using sol–gel and hydrothermal methods. Reprintedwith permission from [298]. Copyright 2025 American Chemical Society.2.7. Nanoarchitectonics of Stacked Macrocycle NanosheetDue to their anisotropic ultra-thinness, 2D nanostructures consisting of monolayers ora few layers exhibit unique properties. Therefore, stacked nanosheet structures are alsointeresting targets for nanoarchitectonics. In their study, ‘Nanoarchitectonics of exfoliatedflexible nanosheet based on laterally stacked macrocycles’, Kim, Oaki and coworkers devel-oped a new type of exfoliated organic 2D material, as shown in Figure 7 [299]. This designdemonstrates nanoarchitectonics involving the synthesis, controlled assembly, polymeriza-tion and exfoliation of macrocyclic diacetylenes. The diversity of molecular motions andconformations of the macrocycles provides potential structural flexibility for the nanosheets.Therefore, similar flexible organic 2D materials can be obtained by exfoliation by designingmacrocycles containing diverse functional molecular units, resulting in the formation ofexfoliable layered structures. Specifically, the self-assembly of designed macrocyclic di-acetylene monomers with chair conformations leads to the formation of stacked structurescontaining vertically aligned, macrocycle-based layers. The exfoliable layered structureis obtained by topochemical polymerization of the diacetylene moieties. Intercalationand subsequent swelling yield nanosheets based on laterally stacked macrocycles in theaqueous phase. This design is expected to lead to soft materials such as liquid crystals, gelsand composites with flexible structures and dynamic functions.2.8. Nanoarchitectonics of Organic NanosheetResearch into nanosheets that exhibit optical functions is also being conducted withinthe field of nanoarchitectonics. High-mobility, ultrathin, 2D organic nanosheets that are onlya few molecular layers thick have attracted considerable attention. However, it is not neces-sarily easy to fabricate ultrathin 2D organic nanosheets that simultaneously possess highluminescence efficiency and flexibility. In a study titled ‘Hierarchical nanoarchitectonics ofultrathin 2D organic nanosheets for aqueous processed electroluminescent devices’, Zhang,Xie and coworkers demonstrated a method for fabricating uniformly sized, ultrathin 2Dorganic nanosheets through multifunctional supramolecular design using a solution-basedtechnique [300]. Specifically, they incorporated methoxyl and diphenylamine groups into3D spiro-fluorene–xanthene building blocks to successfully prepare ultrathin 2D organicnanosheets with a thickness of 19 nm through denser molecular packing, with π-π stackingand CH···π interactions supporting antiparallel and interpenetrating molecular packing indimeric aggregates to favor the formation of ultrathin 2D organic nanosheets. Large-area,Materials 2025, 18, 5196 10 of 36flexible 2D organic nanosheet films were fabricated by a simple drop-coating methodusing an aqueous nanosheet ink. Trimeric aggregates with a 2D brickwork structure wereformed, restricting conformational vibration and rotation, and minimizing nonradiativedeactivation in the solid state. Due to the H-aggregation mode, the resulting ultrathin 2Dorganic nanosheets exhibit stable blue emission and superior photoluminescence quantumyields compared to amorphous films. The crystalline OLED device performance of the 2Dorganic nanosheet films was achieved. These ultrathin 2D organic nanosheets could also beuseful in the development of flexible, electrically pumped lasers and intelligent quantumtunnelling systems.Figure 7. Nanoarchitectonics for exfoliation nanosheets of macrocyclic diacetylenes through self-assembly of designed macrocyclic di-acetylene monomers with chair conformations and topochemicalpolymerization of the diacetylene moieties. Reproduced under terms of the CC-BY license [299].Copyright 2023 Wiley-VCH.2.9. Iron N-Doped Carbon NanoarchitectonicsThe use of nanoarchitectonics in materials development has been widely studied.Nanoarchitectonics for functional carbon materials is a subject of widespread interest. Intheir study, ‘Iron N-doped carbon nanoarchitectonics for C-H bond activation of methy-larenes and esterification reactions’, Gawande et al. reported a method for preparingscalable iron nanoparticles on nitrogen-doped carbon via wet chemical reactions followedby high-temperature pyrolysis [301]. N-doped carbon possesses electron transfer andconductive properties. In particular, its pyridinic-N and graphitic-N compositions make itefficient for synthesizing advanced metal nanomaterials that are useful for organic transfor-mations. The resulting carbon material significantly activates O2 at room temperature togenerate superoxide species. Introducing nitrogen dopants improves the dispersibility andMaterials 2025, 18, 5196 11 of 36stability of Fe nanoparticles and promotes C-H bond activation through the interaction be-tween iron species and nitrogen-containing functional groups. These nitrogen-coordinatediron nanoparticles play an important role as active sites, promoting both toluene oxi-dation and esterification reactions. For instance, when this catalyst is used alongsideN-hydroxyphthalimide, methylarenes can be converted into the corresponding arylalde-hydes with 99% conversion and selectivity at room temperature, without the oxidation ofbenzaldehyde to benzoic acid occurring. Iron nanoparticles decorated with nitrogen-dopedcarbon catalysts could provide durable, easily recoverable and environmentally friendlymetal-based catalysts.2.10. Nanoarchitectonics of Ordered Mesoporous C60–BCNNanoporous and mesoporous materials, which enable the creation of controlled porestructures, are also promising areas of research in nanoarchitectonics. Mesoporous ma-terials, with their unique pore structure and high surface area, hold great potential forenergy storage applications. They have attracted considerable interest as high-performanceelectrode materials for next-generation energy storage devices. In the paper ‘Hybridnanoarchitectonics of ordered mesoporous C60–BCN with high surface area for super-capacitors and lithium-ion batteries’, Vinu et al. synthesized high-surface-area orderedmesoporous hybrids of fullerene and borocarbon nitride (BCN) using KIT-6, a mesoporoussilica with a 3D cage-type porous structure, as a hard template (Figure 8) [302]. The result-ing materials exhibit a high surface area and a uniform distribution of pores, thanks tothe C60 nanostructures decorating the hybrids. This structural feature provides high ioniccharge transport and improved electrochemical stability. Consequently, this nanoporousmaterial demonstrated exceptional performance in energy storage. These materials areconsidered a unique platform for developing highly stable anode materials for energystorage devices. Various advanced spectroscopic tools can be used to analyze the presenceof C60, and applications in novel energy storage systems such as Li+/Na+ hybrid capacitorsand Na+/K+ batteries can be explored. Figure 8. Nanoarchitectonics of high-surface-area ordered mesoporous hybrids of fullerene andborocarbon nitride (BCN) using KIT-6, a mesoporous silica with a 3D cage-type porous structure, as ahard template. Reproduced under terms of the CC-BY license [302]. Copyright 2024 Elsevier.2.11. Nanoarchitectonics: MXene/Covalent Organic FrameworkResearch into nanoarchitectonics is also being conducted using notable materials, suchas MXene nanosheets and covalent organic frameworks (COFs), as components. COFshave excellent adsorbent properties and potential. In order to utilize their capabilities, itis necessary to optimize the stacking/aggregation structure during the synthesis process.In the paper ‘Inorganic–organic nanoarchitectonics: MXene/covalent organic frameworkheterostructure for superior microextraction’, Zhang, Xu, Yamauchi and coworkers de-veloped an inorganic–organic nanoarchitectonics strategy to synthesize an MXene/COFheterostructure (Ti3C2T_x/TAPT-TFP) by assembling β-ketoenamine-linked COFs ontoMaterials 2025, 18, 5196 12 of 36Ti3C2Tx MXene nanosheets (Figure 9) [303]. This material is constructed as follows: First,Ti3C2Tx MXene was ultrasonically dispersed in ethanol under nitrogen bubbling. Sub-sequently, 4,4′,4′’-(1,3,5-triazine-2,4,6-triyl)trianiline (TAPT) monomer was added andallowed to penetrate between the MXene nanosheet layers. Following the covalent linkingof 1,3,5-triformylphloroglucinol (TFP) and the TAPT monomer via a Schiff base condensa-tion reaction, the TAPT-TFP-COF nanostructures assembled on the Ti3C2Tx/TAPT surfaceto form the Ti3C2Tx/TAPT-TFP heterostructure. This material retains the 2D structure andhigh adsorption capacity of MXene, as well as the large specific surface area and hierarchicalporous structure of COF. It also provides a method for synthesizing COF-MXene hybrid ma-terials, which are useful for micro-extracting environmental pollutants. It also enables theextraction of trace organochlorine in fruit and vegetable samples. These materials have beenfound to exhibit low detection limits, wide linearity ranges and acceptable reproducibilityin pesticide analysis. These nanoarchitectonics approaches offer opportunities to addresschallenges in COF nanoengineering through organic–inorganic hybridization strategies. Figure 9. Inorganic–organic nanoarchitectonics strategy to synthesize an MXene/COF hetero-structure (Ti3C2Tx/TAPT-TFP) by assembling β-ketoenamine-linked COFs onto Ti3C2Tx MXenenanosheets. Reproduced under terms of the CC-BY license [303]. Copyright 2024 Wiley-VCH.2.12. Covalent Nanoarchitectonics: Polymer SynthesisNanoarchitectonics involves designing molecular and material structures throughintermolecular interactions, such as hydrogen bonding and electrostatic interactions, aswell as covalent bonds. The synthesis of polymers and related materials is also included innanoarchitectonics research. Polymer synthesis, which involves linking monomer units, isalso considered a nanoarchitectonics process. Indeed, biological systems utilize this strategyadeptly, producing biopolymers with perfectly defined sequences and structures. In thereview paper, ‘Covalent nanoarchitectonics: polymer synthesis with designer structuresand sequences’, Matsumoto et al. introduced notable examples of polymer synthesis withcontrolled sequences and structures from the past and present, including one-dimensionalsequential polymers, multidimensional polymers based on supramolecular template poly-merization and crystal/liquid crystal-based polymerization, and covalent organic frame-works [304]. If these technological and theoretical strategies are realized, artificial polymerswill likely exhibit functionality comparable to that of biological polymers. In particular, theability to easily control the atomic arrangement of polymers would dramatically expandthe available materials library. From a practical viewpoint, polymers play an essentialrole in materials technology, so the development of precisely controlled polymers using ananoarchitectonics approach would be a significant achievement.2.13. Polymer Nanoarchitectonics for Synthetic VesicleIn addition to synthesizing polymers, controlling their assembly structure is alsopart of nanoarchitectonics research. In some cases, this process can mimic biologicalMaterials 2025, 18, 5196 13 of 36structures. In a study titled ‘Polymer nanoarchitectonics for synthetic vesicles with humanerythrocyte-like morphology transformation’, Yoshida demonstrated that synthetic polymervesicles undergo morphological transformations resembling human red blood cells inresponse to temperature changes [305]. The photopolymerization-induced self-assemblyof poly(methacrylic acid)-block-poly(n-butyl methacrylate-random-methacrylic acid) in a70% methanol aqueous solution produced dimpled spherical vesicles that resemble redblood cells. These polymer vesicles exhibited transformation behaviors similar to those ofred blood cells under various conditions. For instance, they transformed into sawtoothor cup-like shapes, resembling red blood cells. The transformations of both the vesiclesand red blood cells were reversible and repeatable. However, repeated cycles resultedin irreversible deformations. The pathways of transformation of the vesicles were alsosimilar to those of red blood cells. Furthermore, synthetic polymer vesicles underwentmorphological changes resembling human red blood cells in response to temperaturechanges. When heated in solution, spherical, red blood cell-like vesicles transformed intoechinocyte-like, sawtooth-shaped vesicles. This occurred as the copolymer constituentswere released from the surface of the vesicles and expanded. As the concentration ofthe vesicles increased, they transformed into cup-shaped vesicles resembling red bloodcells. These observations suggest that synthetic polymer vesicles could facilitate a deeperunderstanding of the unique properties of red blood cell membranes at the molecularlevel. Nanoarchitectonics may elucidate the similarities between living cells and non-livingstructures at the molecular level. This suggests that non-natural polymer vesicles couldsignificantly contribute to our understanding of the causes and mechanisms of intractablediseases, and to their treatment.2.14. Nanoarchitectonics in Colloidal HydrogelThe concept of nanoarchitectonics is also driving the development of advanced col-loidal hydrogels with enhanced functionality for a wide range of applications. In the reviewpaper titled ‘Nanoarchitectonics in colloidal hydrogels: Design and applications in theenvironmental and biomedical fields’, Kim, Kumar and coworkers discuss the technologicallandscape of nanoarchitectonics with a focus on colloidal hydrogels [306]. In particular,integrating nanoparticles and polymers enables the synthesis of multifunctional nanogelplatforms through the chemical or physical crosslinking of nanoparticles, polymers, andsmall molecules. The combined effects of the nanoparticles’ composition, size, shape,structure, binding mechanism, and molecular crosslinker properties largely determinethese synergistic properties. Colloidal hydrogels have great potential for use in biomedicalapplications such as environmental remediation, drug delivery, wound dressings andtherapeutic diagnostics. Nanoarchitectonics in colloidal hydrogels plays an increasinglyimportant role in providing innovative solutions to pressing global challenges in health-care and environmental sustainability. In advanced applications, nanocomposite hydrogelnano-units provide bioelectrical interfaces for signal generation and transduction, enablingthe creation of real-time sensing materials.2.15. Langmuir NanoarchitectonicsResearch into interfacial processes with the nanoarchitectonics concept has madesignificant contributions. In the study, ‘Langmuir nanoarchitectonics: one-touch fabri-cation of regularly sized nano-disks at the air–water interface’, Mori et al. presented amethodology for producing monodisperse, regularly sized disks with thicknesses of sev-eral nanometers and diameters of less than 100 nm, using a Langmuir monolayer as thefabrication medium (Figure 10) [307]. In this method, a monolayer of the amphiphilictriimide tri-n-dodecylmellitic acid triimide is formed on an aqueous phase containing theMaterials 2025, 18, 5196 14 of 36water-soluble macrocyclic oligoamine 1,4,7,10-tetraazacyclododecane (cyclene). In thiscombination, the imide moiety acts as a hydrogen bond acceptor and interacts weakly withthe secondary amine moiety of cyclene, which acts as a hydrogen bond donor. Using theLangmuir–Schaefer method, Langmuir monolayers were transferred onto mica to formdisk-like structures with heights of approximately 3 nm and tunable diameters in therange of tens of nanometers. The use of weak interactions allows for more precise controlof domain size in two dimensions. The organic assemblies are transferred to metallicnanostructures via sputter deposition of metal onto the LB film. The size distributionof the disk-like objects is sufficiently narrow to be within the quantum disk dimension.This enables the fabrication of two-dimensional nanostructures with regular shapes, suchas quantum disks. Controlled fabrication of well-defined nanostructures through a sim-ple macroscopic process that can be carried out at room temperature provides a uniqueapproach to economical, energy-efficient nanofabrication. Figure 10. Nanoarchitectonics methodology for producing monodisperse, regularly sized disks withthicknesses of several nanometers and diameters of less than 100 nm, using Langmuir monolay-ers as the fabrication medium. Reprinted with permission from [307]. Copyright 2012 AmericanChemical Society.2.16. Layer-by-Layer NanoarchitectonicsLayer-by-layer (LbL) assembly is a versatile interfacial process and a promising ap-proach for nanoarchitectonics research. In the study titled ‘Tannic acid facilitated layer-by-layer nanoarchitectonics for hydrophobic conductive cotton fabric with improved stabilityfor thermal management and flexible sensing’, Zeng et al. fabricated conductive cottonfabrics by layering tannic acid and cellulose nanofibre-dispersed carbon nanotubes ontothe fabric surface using the LbL method [308]. First, clean cotton fabrics were alternatelyimmersed in a tannic acid solution and a cellulose nanofiber-dispersed carbon nanotubedispersion to allow self-assembly. Next, the fabrics were immersed in an ethanol solution ofstearic acid to enhance hydrophobicity. Tannic acid and carbon nanotubes exhibit π-π inter-actions, while cellulose nanofibers and tannic acid exhibit hydrogen-bonding interactions.Therefore, tannic acid firmly integrates the cellulose nanofiber-dispersed carbon nanotubesinto the cotton fabrics. Furthermore, the hydrogen-bonding interaction between tannic acidand stearic acid contributes to the coating of stearic acid on the fibers. The strong adhesiveforce of tannic acid fixed the cellulose nanofiber-dispersed carbon nanotubes firmly to thefabric surface. Meanwhile, the stearic acid enhanced the stability of the conductive cottonfabrics, providing excellent resistance to tape peeling, ultrasonic cleaning and water dropletimpact. The hydrophobic, conductive cotton fabrics exhibited excellent electrothermalconversion capabilities and stable thermal performance. Furthermore, they exhibited highMaterials 2025, 18, 5196 15 of 36sensitivity, a fast response time and excellent sensing stability in sensor applications, effec-tively monitoring human body movements such as joint bending, chewing and swallowing.These properties make them promising candidates for energy-efficient heating textiles andtemperature-regulating smart wearable devices. This flexible sensor has excellent breatha-bility and sensing performance, enabling accurate monitoring of physiological activities inpatients. It has great potential for monitoring human health and providing personalizedmedical diagnoses.2.17. Chiral and Topological NanoarchitectonicsNot only does fabricating nanoscale structures with specific topologies confer uniqueproperties on functional materials, but it also has the potential to elucidate the underlyingfunctional mechanisms of many natural systems. The topic of nanoarchitectonics, witha focus on chirality and topology, is fascinating. In the review paper, ‘Emergent chiraland topological nanoarchitectonics in self-assembled supramolecular systems’, Liu andcoworkers outline the progress made in constructing emergent chiral and topologicalnanoarchitectonics using self-assembly methods [309]. The authors focus particularly ontoroids, catenanes, Möbius strips, spirals and fractals. The design of building blocks andvarious self-assembly strategies towards these target structures are also highlighted, outlin-ing feasible approaches to facilitate the tailor-made construction of mesoscopic structures.The integration of chirality into emergent chiral and topological nanoarchitectures in self-assembled supramolecular systems can be achieved through strategies such as symmetrybreaking, topological chirality or the use of enantiopure components. While these studiesdemonstrate great potential, there are significant knowledge gaps in this cutting-edge fieldand further demonstration of functionality and practical applications is essential. Particularattention should be paid to research closely related to chirality and its unique topologicalconfigurations in fields such as mechanical, optical, optoelectronic and magnetic materials.2.18. Nanozyme NanoarchitectonicsNanozymes that mimic the functions of enzymes are also a focus of nanoarchitectonicsresearch. In particular, two-dimensional (2D) nanozymes exhibit properties that mimicenzymes such as peroxidase, oxidase, catalase, and superoxide dismutase. These 2D nano-systems are in increasing demand due to their ability to enable ultrasensitive, label-freedetection, real-time analysis, point-of-care testing and multiplexed biomarker detection.In the review article titled ‘Two-dimensional nanozyme nanoarchitectonics customizedelectrochemical bio diagnostics and lab-on-chip devices for biomarker detection’, Changet al. discuss the advantages of 2D nanozymes and recent advances in their applications inbiosensing [310]. The development of 2D nanozymes with diverse functions offers greatpotential for novel nanozyme-based diagnostic methods and biosensors. The article reviewsthe current status of 2D nanozymes, focusing on their synthesis, biocatalytic activity, andadvances in the development of bio-detection and lab-on-chip devices for cancer andnon-cancer biomarker detection. Further detailed research is required to facilitate theapplication of 2D nanozymes in clinical diagnostics. Notably, integrating wearable devicesfor personalized health monitoring and measuring glucose and albumin biomarkers withIoT/IoMT and AI/ML could provide an attractive solution for automated interpretationof diagnostic results. This advancement could significantly accelerate the adoption ofself-testing and home diagnostic applications.2.19. Biomimetic Chiral Helical NanoarchitectonicsNanoarchitectonics-based material design and creation can also be applied to morepractical uses. One example is the development of therapeutic contact lenses. The challengein developing such lenses is to achieve rapid repair of severe corneal epithelial defectsMaterials 2025, 18, 5196 16 of 36while regulating the oxidative stress environment. In the paper, ‘Bioactive therapeuticcontact lens triggered by biomimetic chiral helical nanoarchitectonics for rapid cornealrepair’, Zhu, Zhao and coworkers designed a bioactive therapeutic contact lens that mimicsthe layered helical structure of the natural cornea [311]. This was achieved by integratingcellulose nanocrystals into poly(hydroxyethyl methacrylate) and forming CeOx on thesurface of the cellulose nanocrystals (Figure 11). This hydrogel has a chiral helical structurethat controls the microenvironment, and the nanoscale CeOx on the surface of the cellulosenanocrystals acts as a reactive oxygen species (ROS) scavenger. This makes the hydrogel abioactive therapeutic contact lens that promotes rapid corneal repair. Experiments usingin vitro and in vivo corneal injury models revealed that this hydrogel has antioxidant,anti-inflammatory and anti-angiogenic properties, enables rapid migration of cornealepithelial cells and contributes to the regulation of the ocular surface microenvironment.This material, which can stimulate cell growth and migration, is expected to be useful infuture corneal tissue engineering applications. Figure 11. Fabrication of bioactive therapeutic contact lens mimicking the layered helical structure ofthe natural cornea upon integrating cellulose nanocrystals into poly(hydroxyethyl methacrylate) andforming CeOx on the surface of the cellulose nanocrystals. Reprinted with permission from [311].Copyright 2025 American Chemical Society.2.20. Nanoarchitectonics of Cello-OligosaccharideBiomolecules, including cellulose, are influential components in nanoarchitectonicsresearch. Recent advances in the nanoarchitectonics of low-molecular-weight cellulose, i.e.,cello-oligosaccharides, have paved the way for the development of artificial nanocellulose.Nanocelluloses composed of cello-oligosaccharides synthesized by enzymatic oligomer-ization or solid-phase glycan synthesis are known as synthetic nanocelluloses. Thesenanostructures are constructed abiotically at the molecular level in a bottom-up man-ner. By adjusting the assembly process and molecular design, the molecular orientation,nanomorphology and surface functionality of artificial nanocellulose can be controlled. Inthe review paper, ‘Nanoarchitectonics of cello-oligosaccharides: a route toward artificialnanocelluloses’, Hata and Serizawa outline the latest research on artificial nanocellulose,from the preparation and self-assembly of cello-oligosaccharides to their potential applica-tions. In contrast to naturally derived nanocellulose, artificial nanocellulose is constructedfrom the bottom up at the molecular level (Figure 12) [312]. The unique properties ofengineered nanocellulose include diverse nano-morphologies, ease of surface function-alization, brittleness, an abundance of terminal glucose residues and the high chemicalpurity of synthetic nanocellulose. Cellulose hydrolysis can produce cello-oligosaccharidesfrom abundant biomass. Further research into the hydrolysis mechanism and productfractionation will enable the production of chemically pure cello-oligosaccharides withcontrolled molecular structures. These properties distinguish engineered nanocellulosefrom naturally occurring nanocellulose in terms of applications. Engineered nanocellulose,Materials 2025, 18, 5196 17 of 36composed of cello-oligosaccharides, is an emerging nanomaterial with diverse applicationsin materials science. Figure 12. Nanoarchitectonics of artificial nanocellulose upon the preparation and self-assembly ofcello-oligosaccharides. Reproduced under terms of the CC-BY license [312]. Copyright 2025 Elsevier.2.21. DNA NanoarchitectonicsDNA is a powerful biomaterial for the rational design and functional enhancement ofnanostructures. Deploying DNA nanoarchitectures at substrate interfaces offers uniqueadvantages that could lead to improved surface properties relevant to biosensing, nanotech-nology, materials science and cell biology. In a Perspective article titled ‘DNA nanoarchitec-tonics: assembled DNA at interfaces’, Howarka outlines the advantages and challenges ofusing assembled DNA as nanoscale building blocks in interfacial layers [313]. He outlinesthree specific applications: homogeneous, dense surface coatings; bottom-up nanopat-terning; and 3D nanoparticle lattices. The first of these is homogeneous films focused onbiomolecular recognition, the second is 2D nanopatterns fabricated by bottom-up methodsand optionally combined with top-down nanofabrication, and the third is 3D nanoparti-cle superlattices. In conclusion, this review emphasizes the potential for future researchinto interfacial DNA nanostructures. DNA nanotechnology at interfaces is a highly in-terdisciplinary field spanning the nanoscale to the microscale, with numerous potentialapplications in the materials and life sciences.2.22. Supramolecular Peptide NanoarchitectonicsPeptides, which can be designed and synthesized in various structures, are alsoa popular subject in nanoarchitectonics research. In the paper, ‘Dual-integrin-targetedsupramolecular peptide nanoarchitectonics for enhanced hepatic delivery and antifibrotictherapy’, Huang, Yan, Zou and coworkers reported the design of self-assembling peptideswith dual integrin-binding motifs for α5β1 and αvβ3 [314]. Incorporating integrin-bindingpeptides into self-assembling building blocks is essential for developing targeted nanoar-chitectonics. By incorporating dual integrin-binding peptides, multifunctionality wasachieved. Using these peptides, this approach demonstrated supramolecular peptidenanoarchitectonics for enhanced liver delivery and antifibrotic therapy. Supramolecularnanoarchitectonics offer high drug loading capacity, favorable structural stability, efficienttargeting and excellent biocompatibility, opening up new avenues for the treatment of liverfibrosis. As integrins are also overexpressed in other fibrotic organs and tumors, the designprinciples of this study can be applied to the development of peptide nanoarchitectonicsfor enhanced targeting and therapeutic efficacy.2.23. Hybrid Nanoarchitectonics with Bacterial ComponentMultifunctional graphene oxide shows promise for use in biomedical applications.Medically effective materials have been fabricated using graphene oxide nanoarchitectonics.In the paper, ‘Hybrid nanoarchitectonics with bacterial component-integrated graphene ox-Materials 2025, 18, 5196 18 of 36ide for cancer photo-thermo-chemo-immunotherapy’, Chintalapati and Miyako developeda bioinspired approach using the cellular components of tumor-isolated Cutibacteriumacnes to enhance the water dispersibility, drug-loading capacity, photothermal conversionefficiency and therapeutic immunogenicity of graphene oxide [315]. This approach enablescamptothecin to target tumors locally with greater effectiveness, while the photothermaleffect of graphene oxide promotes tumor heating. At the same time, Cutibacterium acnescomponents effectively activate the immune system, showing promise for treating advancedcancers. This work improves patient outcomes and paves the way for immune-boostingand nanohybrid-based therapies in oncology. Furthermore, this study contributes to thegrowing interest in nanomedicine and immunotherapy as effective strategies. Functionalgraphene oxide nanohybrids can be spatiotemporally activated by biologically penetratingnear-infrared laser and anticancer drugs, resulting in effective tumor regression in mice.These findings provide a strong foundation for further research toward the optimizationand clinical application of this nanomedicine strategy.2.24. Cell Membrane-Camouflaged NanoarchitectonicsNanoarchitectonics techniques can be used to construct materials with diverse architec-tures, including biomimetic nanoparticles. In the study titled ‘Cell membrane-camouflagednanoarchitectonics of photosensitizer nanoparticles for enhanced phototherapy in surgery’,Zhao, Zhang, Li and coworkers reported on the development of cancer membrane-mimeticnanoparticles composed of chlorin e6 (Ce6) and chlorambucil (CRB) [316]. The hydrophobicchemotherapeutic drug CRB was used to control Ce6 assembly through hydrogen bondingand π-π stacking interactions. The diameter of the nanoparticles could be adjusted from100 nm to 2 µm by altering the reactant-to-solvent ratio. Ce6@CRB nanoparticles exhibitedexcellent photothermal conversion efficiency, twice that of free Ce6. Furthermore, Ce6@CRBnanoparticles could generate singlet oxygen more stably than free Ce6, thereby reducingoxygen dependence. Furthermore, coating the 4T1 cancer membrane on the Ce6@CRBnanoparticle surface conferred homologous targeting ability, improving Ce6 utilization.Additionally, combining photodynamic therapy with photothermal therapy effectivelyactivates the immune system in vivo. Combining phototherapy with surgical resectionminimizes the wound area as much as possible, optimizing both oncological safety and aes-thetics. Interestingly, this treatment involves surgical resection after phototherapy, whicheffectively reduces the wound area. This research provides an effective method of tumorremoval and is expected to be applied to clinical treatment from a patient-centered andhumane perspective.2.25. Liposomal-Based NanoarchitectonicsGenetically engineered lymphocytes incorporating chimeric antigen receptors (CAR Tcells) have enhanced their natural ability to seek out and destroy tumor cells, providingan effective and safe strategy for tumor eradication. However, their efficacy is generallylimited. In their study, ‘Liposomal-based nanoarchitectonics as bispecific T cell engagersin neuroblastoma therapy’, Baeza et al. demonstrated a strategy for targeting CAR Tcells to neuroblastoma cells using nanometric bispecific T cell engagers (Figure 13) [317].In this design, the outer lipid bilayer is decorated with para-aminobenzyl guanidine,which exhibits strong affinity for the norepinephrine transporter that is overexpressed byneuroblastoma cells, as well as for fluorescein, which is recognized by anti-FITC CAR-Tcells. The silica core can access the interior space by fusing with the neuroblastoma cellmembrane via the protocell lipid membrane. These nanometric bispecific T-cell engagerscombine the ability to label neuroblastoma cells with the capacity to deliver therapeuticagents to tumor cells, providing a novel approach to enhancing the efficacy of CAR T-cellMaterials 2025, 18, 5196 19 of 36therapy. These nano-metric bispecific T-cell engagers are modular and easily tunable,allowing them to be adapted to a wide range of malignancies and for use in treatingother solid tumors. This approach can be easily adapted for the treatment of various solidmalignancies and is expected to pave the way for the development of a new family of CART enhancers. Figure 13. Liposomal-based nanoarchitectonics for targeting CAR T cells to neuroblastoma cells usingnanometric bispecific T cell engagers, in which the outer lipid bilayer is decorated with strong affinityfor the norepinephrine transporter as well as for fluorescein, which is recognized by anti-FITC CAR-Tcells. Reprinted with permission from [317]. Copyright 2025 American Chemical Society.2.26. Nanoarchitectonics to Entrap Living CellResearch in nanoarchitectonics has also reported on the use of cells themselves asbuilding materials. In the paper, ‘Nanoarchitectonics to entrap living cells in silica-basedsystems: encapsulations with yolk–shell and sepiolite nanomaterials’, Ruiz-Hitzky andcoworkers used nanoarchitectonics techniques to fabricate biohybrid materials from the bot-tom up for the encapsulation of living cells (Figure 14) [318]. Unicellular microorganisms,namely cyanobacteria and yeast cells, were immobilized in silica- and silicate-based matri-ces organized as nanostructured materials. For instance, bio-nanocomposite-based matricescomprising a combination of chitosan and alginate with sepiolite clay mineral, molded intofilms, beads, or foams, were successfully employed to immobilize cyanobacteria. The silicashell microstructure was found to reduce cell–cell contact. The inorganic matrix enhancedcell viability and maintained bioactivity. Therefore, the efficiency of encapsulation wasimproved compared to methods involving direct contact of cells within a silica matrix. Theencapsulated yeast produced ethanol over several days, suggesting the potential usefulnessof this method as a biocatalyst. This nanoarchitectonics approach could pave the way fornovel biohybrid systems with a wide range of applications, from preserving living cells todeveloping novel whole-cell bio-inorganic catalytic materials.2.27. Cell-in-Catalytic-Shell NanoarchitectonicsNanoarchitectonics encompasses the creation of cell-shell biohybrid structures, whichare formed by encapsulating individual living cells in exogenous materials. These struc-tures have emerged as an exciting new class of functional entities for engineering bio-materials, with properties that extend beyond biochemical modification. In the paper,‘Cell-in-catalytic-shell nanoarchitectonics: catalytic empowerment of individual living cellsby single-cell nanoencapsulation’, Choi et al. presented a simple and flexible approach toimparting exogenous catalytic capabilities to living cells by nano-encapsulating them in asupramolecular metal–organic complex of Fe3+ and benzene-1,3,5-tricarboxylic acid [319].A series of enzymes were embedded in the nanoshells in situ without compromising theirMaterials 2025, 18, 5196 20 of 36catalytic activity. The supramolecular self-assembly of Fe3+ and benzene-1,3,5-tricarboxylicacid generated surface-active species in situ, leading to the spontaneous formation ofnanofilms and shells on almost any substrate, including living cells, while simultaneouslyembedding the enzymes. These nanoshells enhance the catalytic efficiency of multienzymecascade reactions by trapping reactive intermediates within their internal cavities. Nanoen-capsulated cells can acquire exogenous biochemical functions, such as converting toxicchemicals into nutrients. For instance, nanoencapsulated cells can enzymatically degradelethal octyl-β-D-glucopyranoside to D-glucose and possess autonomous cytoprotectivefunctions. This approach could provide a valuable molecular toolkit for combining bio-logical cells with non-natural materials to design next-generation cellular hybrid systems,which show great promise in biomedical and nanobiomedical applications. Figure 14. Nanoarchitectonics techniques to fabricate biohybrid materials from the bottom up for theencapsulation of living cells, in which unicellular microorganisms, namely cyanobacteria and yeastcells, were immobilized in silica- and silicate-based matrices organized as nanostructured materials.Reproduced under terms of the CC-BY license [318]. Copyright 2025 Beilstein Institute.2.28. Machine Learning in NanoarchitectonicsThe final topic is the application of artificial intelligence (AI) techniques, such asmachine learning, in nanoarchitectonics. There is a strong and profound connection be-tween nanoarchitectonics and machine learning. Mathematics has historically played apivotal role in materials synthesis, influencing numerous fields including nanoscience andnanoarchitectonics. In the review paper, ‘Machine learning in nanoarchitectonics’, Skirtachet al. analyze the use of artificial intelligence, machine learning and deep learning in the dis-covery, prediction, optimization, characterization and imaging of nanoarchitectonics [320].Machine learning is commonly used in atomic and molecular science, nanotechnology ofMaterials 2025, 18, 5196 21 of 36colloids and nanofilms, and micro- and macro-engineering, for example. Machine learningis particularly important in nanotechnology for colloids and nanofilms, as nanofabricatedstructures often do not match predicted nanodesigns. This review analyses machine learn-ing approaches, including models and algorithms, and attempts to link them to materialproperties at various scales. This research trend is expected to ultimately lead to the au-tonomous optimization of material properties at different scales. Autonomous synthesisinvolves automating the manufacturing process of materials such as nanoparticles by usingmachine learning algorithms and advanced robotics to streamline and optimize synthesisconditions. Using machine learning models to predict outcomes based on a set of input pa-rameters and experimental conditions enables the rapid identification of optimal synthesisprotocols. For instance, integrating machine learning with automated synthesis platformscan considerably reduce the time and resources needed to produce functional nanomateri-als, such as nanoparticles. Autonomous synthesis requires the development of technologiessuch as machine learning, laboratory automation and robotics, as well as remote connec-tivity, virtual reality tools, and autonomous driving based on these technologies. Suchapproaches hold great promise in advancing the field of nanoarchitectonics.3. Future PerspectivesThis review paper highlights the broad scope of applications of the new concept ofnanoarchitectonics, selecting and discussing recent papers that contain the term ‘nanoar-chitectonics’ in their titles. Rather than attempting to organize them systematically, theselection of papers is broad and diverse, reflecting the wide range of research topics cov-ered. Topics include highly precise structural control at the atomic and molecular level,such as controlling the number of dopant atoms in solid electrolytes, transforming theframework of carbon atoms in carbon materials, developing single-atom catalysts, andcreating nanorobots and microrobots. Various nanomaterials are also included. Examplesof research include functional nanoparticles, nanotubular materials, 2D-organic nanosheetsand MXene nanosheets. Applications of nanostructured functional materials includenanosheet assemblies, nitrogen-doped carbon, nanoporous and mesoporous materials,and nanozymes. Furthermore, polymeric materials engineered through organic chemistry,covalent organic frameworks and vesicle structures constructed from synthetic polymersare also the focus of nanoarchitectonics research. Research is also being conducted intosupramolecular chemistry and controlled structures created by various methods, such aschirality- and topology-controlled structures, chiral helices, Langmuir monolayers, LB films,and LbL assembly. The nanoarchitectonics of biological materials is also a widely pursuedfield of study. Nanocellulose, DNA, peptides and bacterial cell components are used in thisfield. Bio-related nanoarchitectonics also involves creating more complex structures, suchas biomimetic nanoparticles and materials that mimic the lipid membranes of protocells.Research is also being conducted into the organization of living cells themselves and theencapsulation of living cells with exogenous substances. Thus, nanoarchitectonics targetsa very wide range of functional material systems, from atomic and molecular control tocellular structure. The examples presented here are only a small selection, and the scope ofnanoarchitectonics research is extremely broad. Nanoarchitectonics represents a conceptualframework for creating materials at all levels and can be likened to a method for everythingin materials science.In this review, examples are selected with term of nanoarchitectonics in the title.However, many other research approaches can contribute to nanoarchitectonics evenwithout using this terminology. For example, the pulsed laser ablation method and itsvariations are one of the most flexible tools for producing complex nanostructures, includingcore–shell structures, hybrids, and alloys [321,322]. Application of external inputs byMaterials 2025, 18, 5196 22 of 36lasers can provide huge variations of structure modulations in dimensional, phase, andcomposition control through selecting laser parameters, medium type, and processingsequence, which all allow for fine-tuning the functionality of the resulting structureswith optical, magnetic, and catalytic properties. Such combined strategies contributenanoarchitectonics strategies. Not limited to these cases, many existing methods can sharetheir importance with nanoarchitectonics.Here, I would like to focus on the final topic: the application of artificial intelligencetechnology to nanoarchitectonics. This example demonstrates how machine learning andautomated synthesis techniques can contribute to nanoarchitectonics research on func-tional nanoparticles. Introducing AI technology into nanoarchitectonics research will bea significant milestone. Recent research papers have highlighted the contributions of ma-chine learning methodologies to functional materials and various scientific fields [323–328].There is also a growing trend in nanoarchitectonics research towards incorporating AI-related technologies [329–331]. AI technology can be applied to nanoarchitectonics researchin various ways, including optimizing synthesis conditions and using vast amounts of infor-mation to design unprecedented functional materials. As this review shows, the targets ofnanoarchitectonics research are extremely diverse. Using AI technology to create functionalmaterials that cannot be imagined based on experience or rules by incorporating these datasets is a very attractive prospect. Highly functional systems, such as those found in livingorganisms, are coordinated and harmonized in such a way that they exhibit extremely highfunctionality and flexible adaptability [332–334]. We must establish a methodology forcreating such functional material systems. Rather than developing materials specialized ina particular field, we need a development approach similar to that of biological functionalsystems, incorporating a variety of elements. In such an approach, it will be important tointroduce AI technology capable of handling large amounts of information. In addition,strategies with machine learning in nanoarchitectonics for functional materials such asnanoparticles can lead to condition optimization and automatic syntheses. Such approachesenable us to evaluate many possibilities without tedious experimental trials. Introductionof artificial intelligence into nanoarchitectonics approaches has a huge future potential in awide range of target materials and functions.Developing technology that can universally create materials with unexpected functionscould represent the final frontier of materials science. Nanoarchitectonics will play asignificant part in achieving this final frontier in materials science, although several issuesincluding scalability, ethical issues, and reproducibility have to be further considered. So,what kind of functional materials should we ultimately aim for? They should be highlyfunctional systems, similar to those found in biological systems. Photosynthesis, mate-rialtransformation, and signal transduction operate with exceptional efficiency and selectivity.Moreover, these processes occur in an aqueous environment at room temperature andpressure. These highly functional material systems are exactly what we should strive for. Inbiological systems, many functional units work in harmony and are interconnected. Thesefunctional systems are ingeniously constructed within a single system. Developing suchsystems is the ultimate goal of nanoarchitectonics. Biological systems have developed thesesystems over billions of years of evolution. Nanoarchitectonics is based on a comprehensiveconcept that allows for the use of any and all functional materials. 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MDPI and/or the editor(s) disclaim responsibility for any injury topeople or property resulting from any ideas, methods, instructions or products referred to in the content.https://doi.org/10.1080/14686996.2024.2388016https://www.ncbi.nlm.nih.gov/pubmed/39156883https://doi.org/10.1080/14686996.2024.2351356https://www.ncbi.nlm.nih.gov/pubmed/38817247https://doi.org/10.3390/ma18030534https://doi.org/10.3390/ma18010145https://doi.org/10.1002/adma.202107212https://doi.org/10.1007/s11051-022-05535-yhttps://doi.org/10.1002/adma.202510239https://doi.org/10.1126/science.1062023https://doi.org/10.1038/35082000https://doi.org/10.1126/science.1093087 Introduction  Research Target in Nanoarchitectonics from Atom to Living Cell  Nanoarchitectonics for Dopant Atom  Nanoarchitectonics for Pentagon Defect in Carbon  Single-Atom Nanoarchitectonics for Oxygen Evolution Reaction  Single-Atom Nanoarchitectonics for Robotics  Nanoarchitectonics of Nanoparticle  Tubular Nanoarchitectonics  Nanoarchitectonics of Stacked Macrocycle Nanosheet  Nanoarchitectonics of Organic Nanosheet  Iron N-Doped Carbon Nanoarchitectonics  Nanoarchitectonics of Ordered Mesoporous C60–BCN  Nanoarchitectonics: MXene/Covalent Organic Framework  Covalent Nanoarchitectonics: Polymer Synthesis  Polymer Nanoarchitectonics for Synthetic Vesicle  Nanoarchitectonics in Colloidal Hydrogel  Langmuir Nanoarchitectonics  Layer-by-Layer Nanoarchitectonics  Chiral and Topological Nanoarchitectonics  Nanozyme Nanoarchitectonics  Biomimetic Chiral Helical Nanoarchitectonics  Nanoarchitectonics of Cello-Oligosaccharide  DNA Nanoarchitectonics  Supramolecular Peptide Nanoarchitectonics  Hybrid Nanoarchitectonics with Bacterial Component  Cell Membrane-Camouflaged Nanoarchitectonics  Liposomal-Based Nanoarchitectonics  Nanoarchitectonics to Entrap Living Cell  Cell-in-Catalytic-Shell Nanoarchitectonics  Machine Learning in Nanoarchitectonics  Future Perspectives  References