The piezoelectric materials with excellent bioactivity have attracted more attentions recently and have broad potential applications in tissue engineering. In this article, the barium titanate (BT) particles were filled into the polycaprolactone (PCL)/calcium sulfate whisker (CSW) (15 wt%) composites to prepare the PCL/CSW/BT ternary composites. Due to the reinforcement synergy between the CSWs and the BT particles, the mechanical properties of the ternary composites were increased by 50% compared with the PCL/BT binary composites. The piezoelectric coefficient of the ternary composites is still in the range of natural bone. The ternary composite can promote the adhesion and proliferation of cells. The composites in this study have potential applications in tissue engineering.