The amorphous calcium phosphate (ACP)/tricalcium silicate (Ca3SiO5, C3S) composite powders were synthesized in this paper. The exothermal behavior of C3S determined by isothermal conduction calorimetry indicated that the ACP could be synthesis by chemical precipitation method during the induction period (stage II) of C3S. The composite powders were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM) and energy dispersive X-ray spectroscopy (EDS). The results indicated that nanosized ACP particles deposited on the surface of C3S particles to form core-shell structure at pH=10.5, and the nCa/nP of ACP could be controlled between 1.0 and 1.5. The core-shell structure is stable after sintered at 500 oC for 3 h to remove the β-cyclodextrin (β-CD). As compared with the irregular C3S particles (1~5 μm), the composite powders particles are spherical with a diameter of 40~150 μm. Therefore, to obtain the smaller size of composite powders, it is expected to avoid the aggregate of C3S particles in the aqueous solution by addition of dispersant. As compared with C3S, the composite powders may contribute better injectability, strength and biocompatibility.