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The organization of inorganic nanostructures within self-assembled organic or biological templates^,,,,,,,,,, is receiving the attention of scientists interested in developing functional hybrid materials. Previous efforts have concentrated on using such scaffolds^,, to spatially arrange nanoscopic elements as a strategy for tailoring the electrical, magnetic or photonic properties^,,,,,,, of the material. Recent theoretical arguments^,, have suggested that synergistic interactions between self-organizing particles and a self-assembling matrix material can lead to hierarchically ordered structures. Here we show that mixtures of diblock copolymers and either cadmium selenide- or ferritin-based nanoparticles exhibit cooperative, coupled self-assembly on the nanoscale. In thin films, the copolymers assemble into cylindrical domains, which dictate the spatial distribution of the nanoparticles; segregation of the particles to the interfaces …