To improve the corrosion resistance of Mg alloys, composite coatings of layered double hydroxide intercalated with carbonate (LDH-CO 3 , hydrotalcite) particles and magnesium and aluminum hydroxide gel were formed on AZ31 Mg alloy by electrophoretic deposition (EPD) using the LDH-CO 3 suspension with Mg(NO 3 ) 2 and Al(NO 3 ) 3 in total of 1.25125 mmol/L. Wet-dry cyclic corrosion tests were performed for the coated specimens after ultrasonication. LDH-CO 3 particle-rich layer and magnesium and aluminum hydroxide gel-rich layer almost alternately piled up to form a composite layer. The hydroxide gel adhered the particles together and to the substrate. At the bottom of the composite layer, flake-shape LDH-structured substance densely covered the substrate surface. The coverage and thickness of the composite layer increased from sub-micrometers to 30 µm with an increase of Mg and Al ion concentrations of the suspension. By ultrasonication, parts of the composite layer delaminated to expose the LDH-structured substance layer, while the coverage by the remaining composite layer increased with an increase of Mg and Al ion concentrations. The LDH-CO 3 particles and hydroxide gel composite coatings prevented corrosion initiation even in the areas where the LDH-structured substance layer was exposed.