The electrode alloys (Mg1-xZrx)2Ni (x = 0, 0.3) were prepared by mechanical alloying (MA). Mg in the alloy was partially substituted by Zr in order to improve the electrochemical hydrogen storage characteristics of the Mg2Ni-type alloy. The effects of substituting Mg with Zr as well as milling duration on the microstructures and electrochemical performances of the alloys were investigated in detail. The results showed that the substitution of Zr facilitates the formation of amorphous Mg2Ni-type phase. The electrochemical measurement indicated that the substitution of Zr significantly enhances the discharge capacity and cycle stability of the alloys, and it markedly improved the discharge potential characteristic of the alloys. For a fixed alloy, the electrochemical performances, including the cycle stability and the discharge voltage characteristic as well as discharge capacity, of the alloys were markedly improved with prolonging of the ball-milling duration.