Ni-based alloys are considered as the efficient catalyst for hydrogen-storage materials decomposition. Herein, we applied an in-situ melt-quenching method to dope Mo in Ni-based alloy for catalytic hydrogen evolution from hydrogen-storage materials. Importantly, Mo doped Ni-based catalyst exhibits more than 6 times higher TOF value than that of pure Ni both in AB hydrolysis and hydrazine decomposition, because Mo acts as an electron donor to improve the reducibility of Ni. Hydrogen evolution kinetics were studied over a range of temperatures (303-353 K) and initial feed concentrations (catalyst/hydrogen-storage materials (wt/wt) ratios = 0.2-10). Under optimal reaction conditions, the H-2 evolution rate reaches 1.92 mol H-2/(mol(cat) min) and 0.05 mol H-2/(mol(cat) min) in the hydrolysis of ammonia borane and decomposition of hydrazine, which are 6.42 and 6.44 times higher than undoped Ni catalyst, respectively. And the apparent activation energy of ammonia borane hydrolysis and hydrazine decomposition were evaluated to be 26.66 +/- 3.31 kJ/mol and 40.01 +/- 3.38 kJ/mol, respectively. (C) 2020 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.