Hydrogen generation from hydrolysis of the milled At materials in watar at room temperature Is investigated, The hydrolysis mechanism is based oil the work of the microgalvanic cell, where AlOOH (Bohmite) and hydrogen are produced via consumption of Al and water. From the hydrolysis results, the Al-Bi-based materials have better hydrolysis properties than those of the Al-Sn-based materials. Approximately 1000 mL of H, per gram of the Al-Bi-based materials can be generated, and the hydrogen generation rate can be achieved at 160 mL/g/min in the first five minutes of hydrolysis. The high reactivity of the Al-Bi materials conic from the additives (Zn, hydrides, and salts) and can be achieved in 5 h of milling. Meanwhile, the feasibility of the CO2-free hydrogen from At alloys for fuel cell applications is confirmed in pur experiments, and the hydrogen generation can be controlled by feeding the water flow into the At alloys.