Self-assembling polymers as templates for bioinspired materials synthesis is an emerging field. Ionic block copolymers which self-assemble to form macroscopic gels in response to pH and temperature are ideal candidates as templates for biomimetic materials design. In this study, ionic block copolymer micelles in aqueous solutions were used as templates for the growth of calcium phosphate nanocrystals and subsequently allowed to self-assemble to form thermoreversible nanocomposite gels. Pentablock copolymers with zwitterionic and anionic side chains were used as polymer templates in this study. SAXS and SANS measurements along with XRD, NMR, TEM and rheological experiments were performed to study the ordered polymer based nanocomposite superstructure. Scattering measurements indicate ordered polymer-inorganic superstructure with ~ 17 nm nanometer size particles. Solid state NMR further strengthens these findings with indication of closer polymer-inorganic contact with inorganic particle sizes around 20 nm. Rheology measurements showed that these inorganic superstructures strengthen the polymer structure by exhibiting high storage and loss moduli values. To conclude, successful templating was demonstrated by ionic polymer templates for calcium phosphate nanocrystal formation without disrupting the polymer superstructure. The ionic block copolymer templates enable self-assembled nanocomposite synthesis, facilitating a bottom-up approach to materials design and synthesis.