Low Al single-phase magnesium alloy surfaces with dense magnesium oxide films were uniformly formed. The films were deposited with a radio frequency magnetron sputtering process with a planar magnetron sputtering system. The thickness of deposited magnesium oxide thin films was around 240 nm. According to the XRD results, a magnesium oxide phase film was formed on the substrate. The surface was uniform, and no cracks or exfoliation were observed. The deposited magnesium oxide film did not have any cracks or pores, and the surface of the sample was covered by magnesium oxide. The hardness of the magnesium oxide-coated magnesium alloy reached around Hv200, while that of the uncoated Mg-alloy was around Hv80. Moreover, the Vickers indenter under a 10-mN load indented the magnesium alloy substrate coated with the magnesium oxide film to a depth of around 640 nm, while that for the uncoated magnesium alloy substrate was around 620 nm. Meanwhile, the elasticity value for the magnesium alloy substrate coated with magnesium oxide film was around 5.3×1010Pa, while that of the uncoated magnesium alloy substrate was around 4.2×1010Pa.