The present study explored the in-situ deposition of hard and adherent nanocrystalline protective coatings on NiTi/PZT/TiOx thin film heterostructure prepared by dc/rf magnetron sputtering. Protective layers (AlN, CrN and TiCrN) of approximate thickness (~200nm) were used to improve the surface, mechanical and corrosion properties of NiTi/PZT/TiOx heterostructure without sacrificing the shape memory effect and ferroelectricity of the NiTi and PZT layers, respectively. The influence of the protective layer on structural, electrical and mechanical properties of NiTi/PZT/TiOx heterostructure was systematically investigated and the results were compared. Nanoindentation studies were performed at room temperature to determine the hardness and reduced modulus. The surface modified NiTi/PZT/TiOx heterostructures were found to exhibit high hardness, high elastic modulus and thereby better wear resistance as compared to pure NiTi/PZT/TiOx films. From the results of potentiodynamic polarization test conducted in 1M NaCl solution, the CrTiN coated NiTi/PZT/TiOx heterostructure showed the best corrosion resistance with the lowest corrosion current density (1.52×10−8Acm−2) and the highest protective efficiency (96.8%). The results presented here prove the potential of a surface modified NiTi/PZT/TiOx heterostructure to be used in various microelectromechanical (MEMS) applications.