In order to fabricate high efficiency, light-weight hydrogen storage materials in an economical way, we have been made to propose a new mechanical alloying process by high-pressure hydrogen induced planetary ball milling(HIMA) using Mg and Ni chips. Microstructural evaluations of the Mg-Ni-H systems synthesized were investigated by scanning electron microscopy and the transmission electron microscopy. X-ray diffraction analysis was also made to characterize the lattice constant, crystallite size and misfit strain. The hydrogenation properties of the particles synthesized were evaluated by automatic PCI (pressure-composition-isotherm). Adopting 66:1 BCR (ball to chips mass ratio) for HIMA process, fully hydrogenated alloys were obtained after 96 hrs of milling, resulting in total hydrogen content of 2.25 mass%.