To guarantee the long-term stability of an orthopaedic implant, non-degradable surface coatings with the ability to selectively release bioactive drugs or ions are especially desirable. In this study, SrO-TiO composite coatings were deposited on the surface of Ti alloys, whose release behavior of bioactive Sr ions was modulated by the Sr configurations, either interstitial atoms in solid solution (Ti Sr O) or strontium titanate (SrTiO). A perfect linear relationship between the amount of the released Sr ions and the Sr content in the coating was observed. Among the SrO-doped TiO coatings, the 20% SrO-TiO coating where Sr existed in both forms of Ti Sr O and SrTiO not only promoted proliferation of bone cells but also enhanced their osteogenic differentiation, which was proved to be related to its Sr release behavior. However, overdosing with 30% SrO only resulted in one single Sr configuration (SrTiO) and an inferior osteogenic function. This study suggests that Sr configurations of both interstitial atoms of the solid solution and SrTiO can realize the selective release of Sr, but they possibly have different effects on the biological functions and other properties including corrosion resistance.