The design and development of novel materials for biomineralized tissues is an extremely attractive field of research where calcium phosphates (CaPs)-based materials for biomedical applications play a leading role. The biological performance of these compounds can be enhanced through functionalization with biologically active ions and molecules. This review reports on some important recent achievements in creating functionalized biomimetic CaP materials for applications in the musculoskeletal field. Particular attention is focused on the modifications of these inorganic compounds with bioactive ions, growth factors and drugs, as well as on recent trends in some important CaP applications as biomaterials - namely, as bone cements, coatings of metallic implants and scaffolds for regenerative medicine.