Herein we present and discuss the catalytic activity results of nickel-based bimetallic nanoparticles towards the two-step dehydrogenation of hydrazine borane N2H4BH3. Cobalt, iron and palladium were chosen as the second metal, and a series of Ni1-xMx nanocatalysts were prepared by surfactant-aided co-reduction method. The challenge was to find a nanocatalyst that is active in the decomposition of the N2H4 moiety of hydrazine borane. Of the 14 Ni1-xMx combinations, the best results were achieved with Ni0.7Fe0.3 and Ni0.7Pd0.3. At 50 degrees C, 3.9 and 4.3 mol H-2 + N-2 per mole of N2H4BH3 were measured, indicating an activity in the decomposition of the N2H4 moiety. Then, both nanocatalysts were characterized by XRD, SEM, EDX, TEM, SAED and XPS. Finally, the differences in catalytic activity were discussed in terms of electronic and geometric effects. Copyright (c) 2014, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights reserved.