The production of hydrogen through the aluminum‐water reaction has received increasing attention in recent years. In this study, a series of Al‐Ga‐In‐Sn‐KCl composites were prepared by mechanical ball milling for hydrogen generation. The effects of composite composition and preparation process on hydrogen generation are studied. It is determined that the optimal ball milling time for the Al‐6Ga‐2In‐1Sn‐1KCl, Al‐5Ga‐2In‐1Sn‐2KCl, and Al‐4Ga‐2In‐1Sn‐3KCl composites to reach their maximum hydrogen yield is 4, 7, and 9 hours, respectively. In particular, the 7 hours milled Al‐5Ga‐2In‐1Sn‐2KCl composite exhibits the best hydrogen generation properties among all composites, achieving a hydrogen yield of 1127 mL g−1 in pure water at 25°C. The microstructure characterization results show that the intermetallic compound In3Sn is formed in these three composites, and the three composites exhibit different morphologies due to their different compositions and different milling times. The effect of initial water temperature is also studied, and the best milled Al‐6Ga‐2In‐1Sn‐1KCl and Al‐5Ga‐2In‐1Sn‐2KCl composites are completely hydrolyzed as the water temperature rises to 60°C. Due to their good hydrogen production capacity, these composites are expected to become an energy source for real‐time hydrogen supply.