Supported non-noble transition metal catalysts are ideal for use in NaBH4-based hydrogen storage systems because of their low cost, robustness, and ease of handling. We have developed a new low-temperature electroless plating method for preparation of CoeB catalysts supported on Ni foam. This method requires only one plating step to achieve the desired catalyst loading, and has higher loading efficiency than conventional multi-step methods. The produced CoeB catalyst shows higher NaBH4 hydrolysis activity than those prepared by conventional methods due to increased boron content and nanosheetlike morphology. The pH and NH3 concentration of the precursor solution were found to have considerable influences on both the catalyst loading and activity. Temperature dependence of hydrogen generation suggests that the catalytically active phase is formed in situ above a certain temperature threshold, which is supported by XPS analysis. The maximum specific hydrogen generation rate is in excess of 24,000 mL min 1 g 1, which is among the highest values for catalysts of this type reported in the literature.