Magnesium (Mg) and its alloys have been suggested as revolutionary biodegradable materials. However, fast degradation hinders its clinic application. To improve the corrosion resistance and biocompatibility of Mg-Nd-Zn-Zr alloy (JDBM), magnesium-aluminum-layered double hydroxide (Mg-Al LDH) was successfully introduced into Mg(OH)(2) coating by hydrothermal treatment. The anions in the interlayer of Mg-Al LDH can be replaced by chloride ions, resulting in a relatively low chloride ion concentration near the surface of the coating. The favorable corrosion resistance of the coating was proved by polarization curves and hydrogen collection test. The Mg-Al LDH significantly promoted cell adhesion, migration and proliferation in vitro. In addition, the coating almost fulfilled the request of the clinical application in the hemolysis ratio test. Finally, in vivo results indicated that the coating offered the greatest long-lasting protection from corrosion and triggered the mildest inflammation comparing to the pure Mg(OH)(2) coatings and untreated magnesium alloy. Mg(OH)(2) coating containing Mg-Al LDH in the present study shows a promising application in improving anticorrosion and biocompatibility of Mg alloys, and might act as a platform for a further modification of Mg alloys ascribed to its special layer structure.