In order to improve the wear and corrosion resistance of micro-arc oxidation (MAO) coating on a Ti-5Al-1V-1Sn-1Zr-0.8Mo alloy, 0–0.20 g/L graphene was added to the electrolyte to prepare micro-arc oxidation coating. The thickness, roughness, micro-morphology, and composition of the MAO coating were characterized, and the wear and corrosion resistance of the coating was tested and analyzed. The results show that with 0.05 g/L of graphene in the electrolyte, the roughness of the coating decreased from 56.76 μm to 31.81 μm. With the increase in the addition of graphene, the microstructure of the coating became more compact, the diameter of micro-holes and micro-cracks decreased, and the corrosion resistance of the coating improved. The wear tests showed that the mass loss of the coating at the early wear stage (0~100 revolutions) was greater than that at the later stage (100~250 revolutions), and the wear resistance of the coating obtained by the addition of 0.10 g/L of graphene was the highest. With 0.10 g/L of graphene, the adhesion force between the coating and the substrate alloy is the largest, reaching 57.1 N, which is 9.98 N higher than that without graphene. After salt spray corrosion for 480 h, the coating with graphene has better corrosion resistance than that of a graphene-free coating.