Incorporating Sr element in biomaterials for bone implants is an effective way to improve their biological performance, as Sr element has been proved to enhance bone regeneration and depress bone resorption activity. In the present study, we developed a Sr-incorporated dicalcium silicate (C2S) bone cement as a potential candidate for bioactive self-setting bone cement in orthopaedics and stomatology. The Sr-C2S powders containing 0.3–6.8% Sr in molar ratio were prepared by means of chemical co-precipitation, and the results of XRD analysis indicated the incorporation of Sr element into the lattice of C2S. Sr-C2S bone cements, as prepared by mixing the powders with water, have a final setting time of 570 to 594 min, and compressive strength higher than that of C2S bone cement within certain incorporation range. The Sr-C2S bone cements possessed good in vitro bioactivity by inducing apatite formation in simulated body fluid (SBF) within 7 days. Moreover, the proliferation activity of human bone marrow mesenchymal stem cells (hBMSCs) with Sr-C2S bone cements was significantly higher than that with C2S bone cement, and the alkaline phosphatase (ALP) activity of hBMSCs was also enhanced with addition of Sr element in Sr-C2S groups. The Sr-C2S might therefore be a bioactive self-setting material with enhanced biological performance and holds the prospect for application in the bone regeneration area.