Surface treatment and bioactive metal ion incorporation are effective methods for the modification of titanium alloys to be used as biomaterials. However, few studies have demonstrated the use of air-plasma treatment in orthopedic biomaterial development. Additionally, no study has performed a direct comparison between unmodified titanium alloys and air-plasma-treated alloys with respect to their biocompatibility and osteogenesis. In this study, the biological activities of unmodified titanium alloys, air-plasma-treated titanium alloys, and air-plasma-treated strontium-doped/undoped calcium phosphate (CaP) coatings were compared. The strontium-doped CaP (Sr-CaP) coating on titanium alloys were produced by selective laser melting (SLM) technology as well as micro-arc oxidation (MAO) and air-plasma treatment. The results revealed that rapid air-plasma treatment improved the biocompatibility of titanium alloys and that Sr-CaP coating together with air-plasma treatment significantly enhanced both the biocompatibility and osteogenic differentiation of bone marrow mesenchymal stem cells (BMSCs). Overall, this study demonstrated that low temperature air-plasma treatment is a fast and effective surface modification which improves the biocompatibility of titanium alloys. Additionally, air-plasma-treated Sr-CaP coatings have numerous practical applications and may provide researchers with new tools to assist in the development of orthopedic implants.