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Abstract Even after more than two decades of intense studies, the research on self‐assembly processes involving supramolecular interactions between nanoparticles (NPs) is continuously expanding. Plasmonic NPs have attracted particular attention due to strong optical, electrical, biological, and catalytic effects they are accompanied with. Surface plasmon resonance characteristics of plasmonic NPs and their assemblies enable fine‐tuning of these effects with unprecedented dynamic range. In turn, the uniquely high polarizability of plasmonic nanostructures and related optical effects exemplified by surface‐enhanced Raman scattering and red–blue color changes give rise to their application to biosensing. Since supramolecular interactions are ubiquitous in nature, scientists have found a spectrum of biomimetic properties of individual and assembled NPs that can be regulated by the layer of surface ligands coating all NPs. This paradigm has given rise to multiple studies from the design of molecular containers and enzyme‐like catalysts to chiroplasmonic assemblies. Computational and theoretical advances in plasmonic effects for geometrically complex structures have made possible the nanoscale engineering of NPs, assemblies, and supramolecular complexes with biomolecules. It is anticipated that further studies in this area will be expanded toward chiral catalysis, environmental monitoring, disease diagnosis, and therapy.