A novel bioactive vaterite-containing tricalcium silicate bone cement (V5) was successfully synthesized through self hydration and carbonization, by introducing CO2 into the hydration process of Ca3SiO5 (C3S). The purpose of this work is to reduce the adverse effect of the hydration products Ca(OH)2 on the C3S bone cement, and improve further the bioactivity of the C3S bone cement. XRD and FT-IR analysis indicated that vaterite was successfully formed in tricalcium silicate bone cement. The in vitro bioactivity of V5 was investigated by soaking in simulated body fluid (SBF) for various periods (1, 3, 7days), in addition to setting time, compressive strength and cell behavior. The results showed that the V5 could rapidly induce hydroxyapatite (HA) formation. The bio-effects of V5 on MC3T3-E1 osteoblast-like cells were evaluated by studying cell viability, adhesion and proliferation. The CCK-8 assay shows that cell viability on the resulting V5 is improved obviously after through hydration and carbonization. The V5 cement enhanced the higher expression of cell attachment, proliferation and differentiation as compared to V50 cement. SEM results present significant improvement on the cell adhesion and proliferation for cells cultured on the V5. Experimental results demonstrated that, C3S bone cement of containing vaterite has more excellent bioactivity and medium setting time too, suggesting their potential applications in areas such as MC3T3-E1 cell stimulation and bone tissue engineering.