Sodium borohydride (NaBH 4 ) has been widely regarded as the one of most promising further hydrogen (H 2 )generated materials for the safe storage, transportation, and utilization of H 2 . Therefore, the exploration of more efficient catalytic systems for on-demand H 2 evolution via NaBH 4 hydrolysis is critical. Herein, a series of magnetic recyclable cobalt ferrite (CoFe 2 O 4 )-modified transition-metal nanoparticles (including Ru, Pd, Rh, Pt, Ir, and Ag) for the catalytic hydrolytic dehydrogenation of NaBH 4 for H 2 evolution have been developed for the first time. The order of the catalytic activity is Ru > Pd > Rh > Pt > Ir > Ag, indicating that Ru/ CoFe 2 O 4 and Pd/CoFe 2 O 4 are the most active, with turnover frequencies of 421 and 348 mol H 2 •mol cat −1 •min −1 . By comparing with other carriers, we found the key factor to be CoFe 2 O 4 in facilitating H 2 production upon the hydrolytic dehydrogenation of NaBH 4 in this work. KEYWORDS: sodium borohydride (NaBH 4 ), hydrogen evolution, CoFe 2 O 4 , nanoparticles, hydrolysis