NiTi alloy is considered to have great application potential in the fabrication of metal implant materials. However, the NiTi alloy still suffers from some disadvantages, such as poor corrosion resistance and health hazards caused by the release of nickel ions. In order to improve the corrosion resistance of NiTi alloy, a healing composite coating was prepared on NiTi alloys by micro-arc oxidation doped with ZnO nanoparticles and sol–gel sealing with polyacrylamide. The surface morphology, composition, roughness, thickness, and electrochemical performance of the prepared coating were investigated by SEM, EDS, Eddy current thickness gauge, electrochemical workstation, and so on. The adhesion of the prepared coating was also tested using the pull-off method. The results show that compared with NiTi alloy substrate, composite coating of MAO–ZnO@PAM has a dense microstructure, a flatter surface, the largest inner and interfacial charge transfer resistances, outstanding corrosion resistance, and possesses the self-healing ability under the humid condition. [ABSTRACT FROM AUTHOR]