High velocity arc spraying (HVAS) process was used to deposit Al-Ni-Y-Co amorphous and nanocrystalline composite coating on AZ91 magnesium alloy substrate. The microstructure of the coating was characterized using X-ray diffraction (XRD), scanning electron microscopy (SEM) equipped with energy dispersive spectrometer (EDS) and transmission electron microscopy (TEM). The results show that the coating with thickness of 500 mm presents a dense layered structure with low porosity (1.8%). The coating consists of amorphous, nanocrystalline, and crystalline phases. The microhardness was measured by a microhardness tester. The average values of Vickers hardness for the Al-Ni-Y-Co coating, pure Al coating and AZ91 alloys are about HV 0.1 310, HV 0.1 70, and HV 0.1 60, respectively. The electrochemical corrosion resistance of the coating in 5 wt% NaCl aqueous solution was also investigated, and the results showed that the Al-Ni-Y-Co coating exhibits better corrosion resistance than pure Al coating and AZ91 magnesium alloy.