A cold sprayed Al coating on S355 structural steel was processed using a laser remelting (LR). The surface and cross-section morphologies, chemical compositions, and phases of as-obtained Al coating before and after LR were analyzed using a scanning electronic microscope (SEM), energy dispersive spectrometer (EDS), and X-ray diffractometer (XRD), respectively, and their hardness was measured using a micro-hardness tester. The friction-wear behaviors of Al coating before and after LR in 3.5% NaCl solution were conducted to simulate the sand and gravel scouring on its surface in seawater, the effects of wear loads and speeds on the tribological properties of Al coating were analyzed, and the wear mechanisms under different wear loads and speeds were also discussed. The results show that the Al coating after LR is primarily composed of an Al phase and its hardness is 104.66 HV, increasing 54.70 HV than the cold sprayed Al coating. The average coefficient of friction (COF) of cold sprayed Al coating at the wear load of 0.5, 1.0 and 1.5 N is 0.285, 0.239, and 0.435, respectively, while that after LR is 0.243, 0.227, and 0.327, respectively, decreased by 14.73%, 5.02% and 24.83% compared to the cold sprayed Al coating. The wear rate of cold sprayed Al coating at the wear load of 0.5, 1.0 and 1.5 N is 1.60 × 10−4, 2.36 × 10−4, and 2.40 × 10−4 mm3/m·N, respectively, while that after LR is 1.59 × 10−4, 1.70 × 10−4, and 1.94 × 10–4 mm3/m·N, respectively, decreased by 1%, 32%, and 23%, respectively, indicating that LR has high anti-friction performance. Under the wear load action of 1.0 N, the average COF of laser remelted Al coating at the wear speeds of 300, 400 and 500 times/min is 0.294, 0.279, and 0.239, respectively, and the corresponding wear rate is 1.06 × 10−4, 1.24 × 10−4, and 1.70 × 10−4 mm3/m·N, respectively. The wear mechanism of cold sprayed Al coating is primarily corrosion wear at the loads of 0.5 and 1.0 N, and that at the load of 1.5 N is abrasive wear and fatigue wear; while that after LR is abrasive wear and fatigue wear, with no corrosion wear, showing that LR improves its corrosion and wear resistance.