Titanium/dicalcium silicate composite coatings with different ratios (weight ratios as Ca2SiO4: Ti = 3:7, 5:5, 7:3) were prepared by plasma spraying. Effects of titanium addition on coating properties, such as bonding strength, Young’s modulus and dissolution in simulated physiological environment, were studied. Results showed that the bonding strength between coating and Ti-6Al-4V substrate increased with increase of titanium content in the composite coatings. It was explained by the narrowed dissimilarity of thermal expansion coefficients between the coatings and substrates. Degradation of mechanical properties after immersion in simulated body fluid was also studied. The dissolution of dicalcium silicate in the composite coatings resulted in the decrease of bend strength and Young’s modulus of the coatings in the simulated physiological environment. The higher titanium content in the composite coatings, the stabler are the composite coatings in the physiological environment.