Calcium silicate-based cement (CSC) has attracted much interest because of its favourable osteogenic effect that supports its clinical use. Although CSC has antibacterial activity, this activity still needs to be improved when used in an infected bone defect. Natural polyphenols have been considered antimicrobial reagents. To this end, three different types of polyphenols (gallic acid (GA), pyrogallol (PG) and tannic acid (TA)) with different concentrations as a liquid phase were mixed with bioactive calcium silicate to enhance the antibacterial activity of CSC. The setting time, antibacterial activity, and osteogenic activity of CSC were studied. Evaluation of antibacterial ability and reactive oxygen species (ROS) was performed using Gram-negative Escherichia coli (E. coli) and Gram-positive Staphylococcus aureus (S. aureus) bacteria, while a human osteoblast-like cell line (MG63) was used to examine osteogenic activity. The experimental results showed that the addition of polyphenols did not remarkably affect the phase composition and morphology of CSC, but changed the setting time and diametral tensile strength. At the same concentration of 1 wt%, the setting time of TA (21 min) was significantly shorter than that of PG (26 min) and GA (68 min), and was indistinguishable from the control cement (20 min). GA had a significantly higher antioxidant activity than PG and TA. As expected, higher concentrations of polyphenols had a more positive impact on ROS generation. More importantly, the incorporation of polyphenols greatly enhanced the antibacterial activity of CSC against E. coli and S. aureus, but had little effect on the in vitro osteogenic activity of MG63 cells and the cytotoxicity of L929 cells. It was concluded that among the three phenolic compounds, the optimal concentration of the liquid phase in the hybrid cement was 5 wt% TA in terms of setting time, strength, antibacterial activity and in vitro osteogenic activity.