Implant loosening remains a major clinical challenge for osteoporotic patients. This is because osteoclastic bone resorption rate is higher than osteoblastic bone formation rate in the case of osteoporosis, which results in poor bone repair. Strontium (Sr) has been widely accepted as an anti-osteoporosis element. In this study, we fabricated a series of apatite and Sr-substituted apatite coatings via electrochemical deposition under different acidic conditions. The results showed that Ca and Sr exhibited different mineralization behaviors. The main mineralization products for Ca were CaHPO·2HO and Ca(PO) with the structure changed from porous to spherical as the pH values increased. The main mineralization products for Sr were SrHPO and Sr(PO)OH with the structure changed from flake to needle as the pH values increased. The experiment demonstrated that coatings fabricated at high pH condition with the presence of Sr were favorable to MSCs adhesion, spreading, proliferation, and osteogenic differentiation. In addition, Sr-substituted apatite coatings could evidently inhibit osteoclast differentiation and fusion. Moreover, the study indicated that nano-needle like Sr-substituted apatite coating could suppress osteoclastic activity, improve new bone formation, and enhance bone-implant integration. This study provided a new theoretical guidance for implant coating design and the fabricated Sr-substituted coating might have potential applications for osteoporotic patients.