Biomineralization, the process by which organisms create a variety of sophisticated composites such as bone and shell, is an ideal model toward materials fabrication in an environmentally friendly way. This article reviews recent progress in the biomineralization-inspired synthesis of polymer–inorganic composites including (1) polymer–calcium carbonate thin films synthesized by interaction among insoluble polymer, soluble acidic polymer, and inorganic ions; (2) polymer nanogel–calcium phosphate nanoparticles synthesized on scaffolds of hydrogel nanoparticles; and (3) colloidal silica nanoparticles made to self-assemble into anisotropic structures by interaction with block copolymers.