The effects of nickel coating on the electrochemical properties of Mg2Ni hydrogen storage alloys are presented in this paper. X-ray diffraction (XRD) and scanning electron microscope (SEM) techniques were employed to examine the crystal structure and surface morphologies of the bare and Ni-coated Mg2Ni alloys. The electrochemical properties of alloys were characterized by cyclic voltammetry (CV) and electrochemical impedance spectroscopy (EIS). The results showed that Ni coating not only decreased the charge transfer resistance, but also decreased the H atom diflusion resistance for Mg2Ni alloys. It was also found that Ni coating effectively improved the discharge capacity, but decreased the cycling performance of the as-synthesized Ni-coated Mg2Ni alloys. The discharge current has a great impact on the cycling performance of the as-synthesized Ni-coated Mg2Ni alloys.