Magnesium hydride is a potential candidate for storing hydrogen; however, due to its slow kinetics and stable thermodynamics it is difficult to use in real-world applications. In this work, we successfully synthesized different composites of Ni@C with MgH2 to improve its kinetics. Experimental results indicate better performance of all catalyzed samples as compared to the pristine MgH2. Especially, the addition of core-shell structured Ni@C enabled MgH2 to desorb hydrogen at 252 °C, which is 56 °C lower than the milled MgH2. The apparent activation energy of dehydrogenation decreased from 109.2 ± 4.1 kJ/mol (milled MgH2) to 83.1 ± 0.3 kJ/mol (catalyzed MgH2). This kinetic enhancement can be attributed to the synergistic effects of Ni, making dissociation and recombination for hydrogen easier, and the C species, inhibiting particle agglomeration. PCT measurement showed that catalysts did not alter the process thermodynamics. In the cycle stability test of NG3:10: 2, the hydrogen storage capacity was retained at 75 % after 20th cycle and only falls by about 1.6 wt percent. In addition, XRD and SEM demonstrated that the novel species of Ni@C and Mg2Ni/Mg2NiH4 together increased the absorption and dissociation of hydrogen.