Methodology to self-assemble metal nanoparticles into three-dimensional mesoscale patterns is a fundamental technique to construct functional materials. Here, we demonstrate that hybridizing an immiscible polymer pair with a metal nanoparticle allows the hybrid to self-assemble in the film, resulting in spontaneous alignment of the nanoparticles at the phase-separated interface formed by the constituent polymers. Organic–inorganic hybrids ...