<p>We report the development of a novel magnetically separable palladium(0) nanocatalyst for hydrogen generation from the hydrolysis of ammonia borane. Palladium(0) nanoparticles become magnetically separable when supported on the surface of magnetic nickel ferrite (NiFe₂O₄) nanospheres. The borohydride reduction of palladium(II) ions, impregnated on the nickel ferrite, yields the Pd⁰/NiFe₂O₄ nanoparticles which are easily separated from the reaction medium by an exterior magnet and characterized by a combination of advanced analytical techniques. The Pd⁰/NiFe₂O₄ nanocatalyst with a 0.25% wt. Pd content has highly dispersed Pd⁰ nanoparticles of ∼4&#xa0;nm mean size on the surface of NiFe₂O₄ nanopowder. Pd⁰/NiFe₂O₄ nanoparticles are found to have superb activity providing a turnover frequency value of 2270&#xa0;min^− 1 in releasing dihydrogen (H₂) from the hydrolysis of ammonia borane (AB) at 25.0&#xa0;°C. Thanks to their magnetic isolability Pd⁰/NiFe₂O₄ nanoparticles also provide outstanding reusability as they retain the complete initial activity even after tenth run of hydrolysis of AB releasing 3 equivalent H₂ gas per mole of AB; that is, 100% conversion. The high activity and outstanding stability of the magnetically isolable Pd⁰/NiFe₂O₄ nanoparticles are ascribed to the favorable interaction of palladium with the oxide surface of NiFe₂O₄, as elucidated by the X-ray Photoelectron Spectroscopy. The strong interaction of palladium with the oxide support can keep the nanoparticles tightly bound on the NiFe₂O₄ surface. More importantly, such a metal-support interaction facilitates the charge transfer from palladium nanoparticles to oxide surface, which causes a significant enhancement in catalytic activity.</p>