Nanoparticles drive self-limiting nanostructure assembly

• New assembly strategy for colloidal nanostructures inspired by natural self-limiting processes. • Cucurbituril (CB) acts as molecular ‘glue’ for InP/ZnS quantum dots (QDs) and plasmonic Au nanoparticles. • InP/ZnS QDs control self-assembly of larger plasmonic nanoparticles via interfacial self-limiting aggregation (ISLA). • Self-assembled nanostructures could enable next generation optoelectronics, drug delivery, sensing and nanotheranostics.