Science in the small world has become a crucial key that has the potential to revolutionize materials technology. This trend is embodied in the postnanotechnology concept of nanoarchitectonics. The goal of nanoarchitectonics is to create bio‐like functional structures, in which self‐organized and hierarchical structures are working efficiently. Liquid–liquid interface like environments such as cell membrane surface are indispensable for the expression of biological functions through the accumulation and organization of functional materials. From this viewpoint, it is necessary to reconsider the liquid–liquid interface as a medium where nanoarchitectonics can play an active role. In this review, liquid–liquid interfacial nanoarchitectonics is classified by component materials such as organic, inorganic, carbon, and bio, and recent research examples are discussed. Examples discussed in this paper include molecular aggregates, supramolecular polymers, conductive polymers film, crystal‐like capsules, block copolymer assemblies, covalent organic framework (COF) films, complex crystals, inorganic nanosheets, colloidosomes, fullerene assemblies, all‐carbon π‐conjugated graphite nanosheets, carbon nanoskins and fullerphene thin films at liquid–liquid interfaces. Furthermore, at the liquid–liquid interface using perfluorocarbons and aqueous phases, cell differentiation controls are discussed with the self‐assembled structure of biomaterials. The significance of liquid–liquid interfacial nanoarchitectonics in the future development of materials will then be discussed.