The surface structure and high specific surface area affect electrochemical response of partially oxidized porous NiTi nanostructure in energy storage and corrosion protection. NiTi nanostructure was synthesized by mechanical alloying of the elemental Ni and Ti powders with a high energy ball milling at a stainless steel vial under an argon atmosphere. Particularly, FTIR spectrum shows that a variety of the functional groups and Ni and Ti oxides on the surface of the particles have been produced. X-ray diffractometer and transmission/scanning electron microscopy techniques are used to investigate the microstructure of the milled powder and electrochemical techniques are used to evaluate electrochemical properties. The partially oxidized NiTi alloy has capacitance of 60 F g− 1 in 6 M of KOH and 80 F g− 1 in 1 M Na2SO4 at different current densities, demonstrating the importance of NiTi in the charge transfer.