Nowadays, the majority of the commercially available calcium phosphate materials is fabricated by 'classical' materials science approaches, i.e., from rather poorly defined slurries or from organic solvents, often at high temperatures and pressures. Bioinspired precipitation of inorganics with (polymeric) additives from aqueous solution, on the other hand, enables the synthesis of intriguing inorganic or organic/inorganic materials that are often much more closely related to biological structures. This article discusses approaches for the fabrication of bio-inspired calcium phosphate hybrid materials by precipitation from aqueous solution. The article focuses on polymers and related self-assembling structures for the design of CaP/organic hybrids and pure CaP with crystal structures and morphologies regulated by the respective additive.