The effect of partial substitution of Al and Mo for Ni on the structure and electrochemical properties of the La0.7Mg0.3Ni3− x (Al0.5Mo0.5) x (x =0–0.4) hydrogen storage alloys have been investigated systematically. The result of X-ray powder diffraction (XRD) and Rietveld analysis show that all the alloys consist of the La(La, Mg)2Ni9 phase and the LaNi5 phase. Meanwhile, the lattice parameter and the cell volume of both the La(La, Mg)2Ni9 phase and the LaNi5 phase increase with increasing Al and Mo contents in the alloys. The pressure composition isotherms curves indicate that the hydrogen storage capacity first increases and then decreases with increasing x. The electrochemical measurements show that the maximum discharge capacity of the alloy electrodes first increases from 343.3 (x =0) to 377.6mAh/g (x =0.3) and then decreases to 350.4mAh/g (x =0.4). Moreover, the high rate dischargeability (HRD) and the exchange current density of the alloy electrodes decrease first and then increases with the increase of x in the alloys. The hydrogen diffusion coefficient increases with increasing Al and Mo content and thus increases the low temperature dischargeability (LTD) of the alloy electrodes.