In order to improve the poor comprehensive performance of aluminum bronze surface, a duplex surface modification technology consisting of laser cladding and followed by plasma nitriding was adopted to prepare the infiltration composite modified layer. The effects of different surface treatment techniques on the microstructure and properties of the modified layer were investigated. The results show that the laser cladding surface is mainly composed of Cu-rich intermetallic compounds, and the AlN layer appears on the surface after plasma nitriding treatment, which significantly improves the hardness and tribological properties. The surface modification treatment changes the surface morphology. The microhardness of the alloy surface after composite modification is much higher than that of untreated and single treatment. It is about six times that of the Cu-Al matrix. At the same time, the composite modified layer has a lower friction coefficient and wear volume, showing excellent tribological properties. These research results can provide a new way for the surface design and development of metal materials.