Calcium phosphate-AMP layered material was synthesized by the hydrolysis of α−TCP in the presence of AMP at pH=6.2. The resulting composite was a mixture of DCPD and calcium phosphate-AMP layered material. The composition and structures of the calcium phosphate-AMP layered material were estimated based on elemental analysis, thermal analysis, and spectroscopic analyses. About 30 wt% of the composite comprises AMP, which is oriented in alternately layered structure of AMP and calcium phosphate layers. Furthermore, the composite showed better cell adhesion than DCPD.