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Precise control of the spatial organization of nanoscopic building blocks, such as nanoparticles, over multiple length scales is a bottleneck in the ‘bottom-up’ generation of technologically important materials. Only a few approaches have been shown to achieve nanoparticle assemblies without surface modification. We demonstrate a simple yet versatile approach to produce stimuli-responsive hierarchical assemblies of readily available nanoparticles by combining small molecules and block copolymers. Organization of nanoparticles into one-, two- and three-dimensional arrays with controlled inter-particle separation and ordering is achieved without chemical modification of either the nanoparticles or block copolymers. Nanocomposites responsive to heat and light are demonstrated, where the spatial distribution of the nanoparticles can be varied by exposure to heat or light or changing the local environment. The …