Calcium silicate-based cements are known for their wide applications in dentistry and orthopedics. The alkaline pH (up to 12) of these cements limits their application in other orthopedic areas. In this study, the effect of dicalcium phosphate dihydrate (DCPD) coating on set cement on pH reduction and biocompatibility improvement was examined. Samples with 0 and 10 weight ratio DCPD were prepared and characterized by XRD, FTIR, and SEM. The DCPD coating on the set cement was performed by a 7 d immersion in 1% monocalcium phosphate (MCP) solution and characterized by XRD, FTIR, SEM, and EDX. Also, the compressive strength and cytotoxicity of the samples were tested. The results showed that DCPD coating did not significantly change the compressive strength of the cement, but by decreasing the pH of the culture medium to the physiological range, it led to enhance adhesion, spreading and proliferation of human osteosarcoma cell line (Saos-2). The novel DCPD coated calcium silicate-based cement could be served as a bulk or porous bone substitute and scaffold.