The crystal structure, hydrogen storage property and electrochemical characteristics of the La0.7Mg0.3Ni3.5− x (Al0.5Mo0.5) x (x =0–0.8) alloys have been investigated systematically. It can be found that with X-ray powder diffraction and Rietveld analysis the alloys are of multiphase alloy and consisted of impurity LaNi phase and two main crystallographic phases, namely the La(La, Mg)2Ni9 phase and the LaNi5 phase, and the lattice parameter and the cell volume of both the La(La, Mg)2Ni9 phase and the LaNi5 phase increases with increasing Al and Mo content in the alloys. The P–C isotherms curves indicate that the hydrogen storage capacity of the alloy first increases and then decreases with increasing x, and the equilibrium pressure decreases with increasing x. The electrochemical measurements show that the maximum discharge capacity first increases from 354.2 (x =0) to 397.6mAhg−1 (x =0.6) and then decreases to 370.4mAhg−1 (x =0.8). The high-rate dischargeability of the alloy electrode increases lineally from 55.7% (x =0) to 73.8% (x =0.8) at the discharge current density of 1200mAg−1. Moreover, the exchange current density of the alloy electrodes also increases monotonously with increasing x. The hydrogen diffusion coefficient in the alloy bulk increases with increasing Al and Mo content and thus enhances the low-temperature dischargeability of the alloy electrode.