NiTi alloys have been intensively applied in biomedical fields because of their unique intrinsic properties. However, the high content of nickel of NiTi alloys is the major concern on their applications of biomedical fields. In addition, the postoperative infections still may be occurred due to the intrinsic unsatisfied antibacterial activity of NiTi. To overcome the above barriers, a silver-polydopamine (Ag/Pdop) composite film was covered on NiTi surface. The modified NiTi exhibited much better antibacterial and corrosion resistance properties than that of the polished NiTi but higher cell toxicity to human bone mesenchymal (hBMSCs). In order to improve the cytocompatibility, a second polydopamine (Pdop) film was coated on Ag/Pdop, forming a novel sandwich like Pdop/Ag/Pdop composite film. Despite the Pdop/Ag/Pdop exhibited a weaker antibacterial performance than that of Ag/Pdop, its cytocompatibility enhanced obviously. In addition, the Pdop/Ag/Pdop modified NiTi showed a better corrosion resistance than that of the Ag/Pdop. The above excellent properties made the Pdop/Ag/Pdop modified NiTi more suitable for biomedical fields.