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Mg hydride has a relatively high hydrogen storage amount of 7.6wt%, and inexpensive due to abundant resources, but has high reaction temperature and long reaction time because of treble oxidation reactivity and upper activation energy. Their range of applications could be further extended if their hydrogenation kinetics and degradation behavior could be improved. Therefore, the effect of CaO has improved the hydrogenation kinetics and slowed down the degradation. This study focused on investigating whether to improve the hydrogenation kinetics by synthesizing Mg2NiHx-5wt% CaO composites. The Mg2NiHx-5wt% CaO composites have been synthesized by hydrogen induced mechanical alloying. The synthesized composites were characterized by performing X-ray diffraction, Scanning Electron Microscopy, Brunauer–Emmett–Teller, Thermogravimetric, and Sivert's type automatic pressure–composition–temperature analysis. Hydriding kinetics were performed using an automatic PCT measurement system and evaluated over the temperature range of 423 K, 523 K, and 623 K. As a result of calculating the hydrogen adsorption amount through the hydrogenation kinetics curve, it was calculated as about 0.42wt%, 0.91wt%, and 1.15wt%, the highest at 623 K and the lowest at 423 K.