Hybrid nanoparticle (NP) arrays based on particles of different sizes and chemistries are highly desirable to obtain tunable properties for nanodevices. A simple approach to control the spatial organization of NP mixtures within supramolecular frameworks based on NP size has been developed. By varying the ratio of the NP size to the periodicity of the block-copolymer-based supramolecule, a range of hybrid NP assemblies in thin films, ranging from 1D chains to 2D lattices and 3D arrays and networks of NPs, can be readily generated.