In this work, a Cu foil supported array of leaf-like Co₃Ni microstructures composed of well aligned nanorods was synthesized by a facile electroless process. It was found that the as-prepared Co₃Ni array exhibited ferromagnetic properties with enhanced coercivity. The static contact angle of water on the surface of the Co₃Ni array could reach 154.7°, indicating that the Co₃Ni array displayed superhydrophobic properties. In addition, the as-prepared Co₃Ni array showed high catalytic activity in the hydrolysis of ammonia borane for hydrogen generation. More importantly, the Co₃Ni array catalyst still retained ca. 91% of its original catalytic activity after 6 cycles, exhibiting significantly improved recyclability and reusability in contrast to many nanocatalysts reported in the literature. The high catalytic performance, together with its ferromagnetic and superhydrophobic properties, makes the Co₃Ni array a multifunctional material with wide applications in different areas.