Destabilized by aluminum hydride, the dehydrogenation properties of ammonia borane (AB) can be improved significantly, including enhanced dehydrogenation kinetics, reduced induction period and suppressed formation of volatile byproducts. Furthermore, a lowered dehydrogenation temperature was also achieved for AlH3, indicating a mutual dehydrogenation enhancement for both AB and AlH3 in this mixture. The destabilized sample, 3AB/AlH3,can totally release more than 12 wt% of high-pure hydrogen (>99 wt%) without any detectable by-products below 250 degrees C. Mechanism investigations indicated that the mutual dehydrogenation enhancement in the mixture is attributed to the Coulombic attraction between the hydridic H delta- in AlH3 and the protonic H delta+ in the NH3 group of AB. Copyright (C) 2014, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights reserved.