Calcium Titanate (CaTiO3) has been introduced as an attractive biomaterial for the enhancement of calcium phosphate deposition in vivo and in vitro. We hypothesized that CaTiO3 directly coated on titanium (Ti) by metal-organic chemical vapor deposition (MOCVD) could be a suitable candidate for biocompatible coatings for medical devices, particularly dental implants. To prove this hypothesis, surface characterization, cell culture, and animal study were completed in this study. The result of this study showed that CTO 800, a CaTiO3 film prepared by heating at 800 °C, had a high hydrophilic surface. Mouse bone marrow stromal ST-2 cells cultured on substrates and CTO 800 exhibited cell differentiation, represented by alkaline phosphatase activity, compared with cells cultured on non-coated Ti and CTO 700 (a CaTiO3 film prepared by heating at 700 °C). The push-in test value of CTO 800, a parameter that indicates the degree of osseointegration, was significantly higher than that of Ti. Calcium titanate coated on Ti by MOCVD has the potential to accelerate the process of osseointegration; thus, our results support the use of CaTiO3 coating for biocompatible biomaterial for medical applications, particularly dental implants.