Multiple advantages, such as good formability, high specific strength, excellent thermal conductivity, and high corrosion resistance, enable aluminum alloy wide application in various fields; however, low surface hardness and poor wear resistance limit its further development. In this study, three surface modification coatings were successfully prepared on the surface of 7A04 aluminum alloy by microarc oxidation (MAO) and a combination of hard anodizing treatment (HA) and physical vapor deposition (PVD), named MAO, HA+W+DLC, and HA+Ti+ta-C, respectively. The microstructure, hardness, and tribological properties of the three coatings and the 7A04 aluminum alloy substrate were studied. The results show that the surface quality and hardness of the coated samples were higher than those of the 7A04 aluminum alloy and that the HA+Ti+ta-C coating possessed the highest hardness of 34.23 GPa. Moreover, the wear resistance of the two multilayer coatings was significantly improved during the ring-block wear tests under oil lubrication, exhibiting a wear rate of 1.51 × 10−7 mm3/N·m for HA+W+DLC and 1.36 × 10−7 mm3/N·m for HA+Ti+ta-C.