The application of carbon cloth (CC) as the catalyst substrate has been gradually concerned because of its novel physical and chemical properties. Herein, Co-Mo-B nanoparticles grown on CC to form film samples (denoted as Co-Mo-B/CC-F) were prepared, characterized, and applied as effective catalysts for catalyzing the ammonia borane (NH3BH3) hydrolysis. The synthesized Co-Mo-B/CC-F sample at pH = 11.5 shows exceptional catalytic properties, including a fast hydrogen generation rate of 3916.1 mL.min(-1).g(-1) at room temperature of 298 K, and an extremely low activation energy of 25.2 kJ mol(-1). The experimental results indicate that the stacked spherical structure, as well as the synergism between bimetal Co-Mo and nonmetal boron, may bring about the improved catalytic properties of Co-Mo-B/CC-F catalyst. Further investigation about the thermodynamic property has shown that Gibbs free energy of activation is reckoned to be 77.6 kJ. mol(-1), demonstrating that NH3BH3 hydrolysis is a non-spontaneous reaction in the presence of Co -Mo-B/CC-F catalyst. This study illustrates that the stacked Co-Mo-B/CC-F catalyst has prosperous application in the non-noble metal catalyst field for the dehydrogenation from NH3BH3. (C) 2020 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.