Magnesium hydrides (MgH2) have drawn a lot of interest as a promising hydrogen storage material option due to their good reversibility and high hydrogen storage capacity (7.60 wt.%). However, the high hydrogen desorption temperature (more than 400 °C) and slow sorption kinetics of MgH2 are the main obstacles to its practical use. In this research, nickel zinc oxide (Ni0.6Zn0.4O) was synthesized via the solid-state method and doped into MgH2 to overcome the drawbacks of MgH2. The onset desorption temperature of the MgH2–10 wt.% Ni0.6Zn0.4O sample was reduced to 285 °C, 133 °C, and 56 °C lower than that of pure MgH2 and milled MgH2, respectively. Furthermore, at 250 °C, the MgH2–10 wt.% Ni0.6Zn0.4O sample could absorb 6.50 wt.% of H2 and desorbed 2.20 wt.% of H2 at 300 °C within 1 h. With the addition of 10 wt.% of Ni0.6Zn0.4O, the activation energy of MgH2 dropped from 133 kJ/mol to 97 kJ/mol. The morphology of the samples also demonstrated that the particle size is smaller compared with undoped samples. It is believed that in situ forms of NiO, ZnO, and MgO had good catalytic effects on MgH2, significantly reducing the activation energy and onset desorption temperature while improving the sorption kinetics of MgH2.