A zinc-aluminum layered double hydroxides (Zn-Al LDHs) film was prepared on AZ91D magnesium (Mg) alloy substrate by electrochemical deposition method. The characteristics of the film were investigated by X-ray diffraction (XRD), Fourier transform infrared (FT-IR) and scanning electronic microscope (SEM). It was found that the electrodeposited film was composed of crystalline Zn-Al LDHs with nitrate intercalation. The Zn-Al LDHs film was uniform and dense though there also presented some small flaws and cracks. The cross cut tape test showed that the film adhered well to the substrate. Polarization and EIS measurements revealed that the LDHs coated Mg alloy had better corrosion resistance compared to that of the uncoated one in 3.5 wt.% NaCl solution, indicating that the Zn-Al LDHs film could effectively protect Mg alloy from corrosion.