In the current study, a sol-gel-synthesized tricalcium magnesium silicate powder was coated on Ti-6Al-4V alloys using plasma spray method. Composition of feed powder was evaluated by X-ray diffraction technique before and after the coating process. Scanning electron microscopy and atomic force microscopy were used to study the morphology of coated substrates. The corrosion behaviors of bare and coated Ti-6Al-4V alloys were examined using potentiodynamic polarization test and electrochemical impedance spectroscopy in stimulated body fluids. Moreover, bare and coated Ti-6Al-4V alloys were characterized in vitro by culturing osteoblast and mesenchymal stem cells for several days. Results demonstrated a meaningful improvement in the corrosion resistance of Ti-6Al-4V alloys coated with tricalcium magnesium silicate compared with the bare counterparts, by showing a decrease in corrosion current density from 1.84 μA/cm2 to 0.31 μA/cm2. Furthermore, the coating substantially improved the bioactivity of Ti-6Al-4Valloys. Our study on corrosion behavior and biological response of Ti-6Al-4V alloy coated by tricalcium magnesium silicate proved that the coating has considerably enhanced safety and applicability of Ti-6Al-4V alloys, suggesting its potential use in permanent implants and artificial joints.