Al2Ga)-xIn (x = 0, 2, 4, 6, 8 wt%) ternary aluminum (Al) alloys with different weight ratio of In for hydrolysis H 2 generation were prepared by meltingcasting technique. The phase compositions and microstructures of Al-rich alloys were investigated by X-ray diffraction (XRD) and high resolution scanning electron microscope (HR-SEM) equipped with an energy dispersive spectrometer (EDS). The effect of In addition ratio on microstructures and H 2 generation performance were investigated, and the hydrolysis mechanism for Al-Ga-In ternary Al-based alloys has been proposed. Al phase as matrix phase in the Al-Ga-In ternary alloy mainly determines the hydrolysis behavior, and the second phase In strongly promotes the hydrolysis process. The increase of In content can accelerate the H 2 generation rate as well as the final capacity and generation yield in neutral water. The generation yields for (Al2Ga)-x In (x = 2, 4, 6, 8 wt%) alloys at 50°C are 0.56, 0.59, 0.62, and 0.66, respectively. The raising hydrolysis temperature can elevate the initial hydrolysis rate, final H 2 generation capacity, and yield. The H 2 generation capacities of (Al2Ga)-8In alloy at 50°C, 60°C, and 70°C are 262, 290, and 779 mL·g −1 , respectively.