A novel material for hydrogen generation with high capacity of H-2 generation has been successfully prepared by ball milling the mixture of Al and home-made fresh Li3AlH6 powder. Its theoretical capacity of hydrogen released is higher than that of pure Al. Results obtained have shown conversion efficiency of Al-Li3AlH6 composite can be close to 100% by increasing the content of Li3AlH6. When the content of Li3AlH6 is 20 wt%, the maximum hydrogen generation rate and hydrogen yield are 2737.6 mL g(-1) min(-1) and 1513.1 mL g(-1), respectively, at room temperature. By XRD, SEM analyses and reaction heat measurements, it demonstrates that the additive Li3AlH6 can provide an additional source of H-2 and an alkaline environment (MOH) as well as additional heat to promote the Al/H2O reaction. Therefore, the Al-Li3AlH6 composite has a very high activity and high capacity of hydrogen released. Copyright (C) 2014, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights reserved.