In this study, surface-metallized CNT (Ni-Cu-CNT)/Cu composite coatings were deposited on a Cu substrate by using the laser-assisted low-pressure cold spraying technique. The microstructure and wear resistance of the composite coatings were studied. The results show that under laser irradiation, significant plastic deformation occurs in the Ni-Cu-CNT reinforcement phase and Cu bonding owing to thermal softening. Ni-Cu-CNT particles are embedded into the plastic-deformed Cu particles to form a continuous, dense, and well-bonded composite coating. The thickness of the composite coating can reach 2609 μm, and the CNTs are uniformly distributed in the composite coating while maintaining its structural integrity. The composite coating with Ni-Cu-CNTs shows excellent wear resistance, the average friction coefficient reduces to 0.385, and the volume wear rate reduces to 1.49×10^-4 mm³/(N·m). Moreover, the Ni-Cu-CNT reinforcing phase in the composite coating reduces the wear of the coating by bearing the load of the grinding ball on the coating surface. In addition, Ni-Cu-CNTs separate from the coating to form a lubricating layer on the coating surface during the wear process, reducing the friction coefficient of the coating, and, thus, improving the wear resistance of the composite coating.