We have developed novel hydroxyapatite (HAp) cement, “chelate-setting HAp cement” on the basis of chelate bonding of inositol hexaphosphate (IP6). In order to create the cement with enhanced bioactivity, we used a silicon-substituted hydroxyapatite (Si-HAp) as a starting material instead of pure HAp powder. The Si-HAp powders were prepared via an aqueous precipitation reaction and surface-modified with IP6 (IP6-Si-HAp). The Si-HAp were synthesized with desired Si contents (0, 0.4, 0.8, 1.6, and 2.4 mass%). Regardless of the amount of Si, the XRD patterns and FT-IR spectra of the powders were similar to each other. Additionally, chemical composition of Si-HAp powders were the almost same as the nominal one. The substitution of Si resulted in a decrease in the a-axis and increase in the c-axis of unit cell of HAp. While, the compressive strength of IP6-Si-HAp cements was higher than that of Si-HAp cements. These results suggest that surface-modification of any powders with IP6 is effective for enhancement of mechanical property. Comparison of mechanical property between HAp and Si-HAp cement specimens revealed that the substitution of lower levels of Si into0 HAp lattice did not greatly influence compressive strength. However, the substitution of high dose of Si (over 2.4 mass%) reduced the compressive strength. Therefore, to fabricate the chelate-setting cements with enhanced bioactivity, it is necessary to control the amount of Si.