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Hydrogen production via Al-H 2 O reaction has potential uses in the fields of space thrusters, engines, and hydrogen fuel cells, where hydrogen production performance of Al-based composites is critical. In this study, low-cost active additives, including g-C 3 N 4 (CN) and NaCl were added to Al−In−Sn (AlIS) alloys by the mechanical ball milling method in order to substitute metal Ga and regulate the hydrogen production activity, as Ga not only increases the cost of Al-based materials but also adversely affects the recycling of products. The results demonstrate that both CN and NaCl additives can effectively enhance hydrogen production performance of AlIS in a single additive system. Further, when 5 wt % of CN and 2.5 wt % of NaCl are concurrently introduced, Al-based composites exhibit the highest hydrogen production efficiency of 94.45% at ambient temperature. The highest hydrogen production rate reaches 475 mL•s −1 •gAl −1 . Even at 2 °C, there is still 86.66% conversion efficiency. The hydrolysates of the Al-H 2 O reaction are composed of Al(OH) 3 and AlOOH, which are primarily influenced by the reaction temperature and the types of Al-based composites. The hydrolysate formation mechanism is analyzed and proposed.