We have developed new nanocomposites formed completely by self-assembly. We have designed polymers that act as templates for growth of calcium phosphate nanocrystals in solution. The polymers subsequently self-assemble in response to temperature to form gels and solids, even in the presence of the inorganic phase. Our studies with solid-state NMR and small angle X-ray scattering have provided insights into the structure and composition of the polymer-inorganic hybrids. Since the nanocrystals coat the polymer micelles prior to gel formation, the structural organization of the polymer gel is maintained even in the presence of the inorganic phase, enabling a bioinspired bottom-up approach to nanocomposite synthesis.