For many years, the Mg-Ni alloys have been studied as good lightweight hydrogen storage materials, however, the alloys present strong difficulties in the fabrication process of mass products. The rotation-cylinder method (RCM) has been developed for magnesium based composites with moderate rotation under a normal atmosphere. In this study, the Mg-3, 6, 9, 12 mass%Ni alloys were easily manufactured by RCM and their hydrogenation properties were evaluated with a Sieverts-type automatic pressure-composition-isotherm (PCI) apparatus at 523, 573 and 623K. The evolution of the microstructure of as-cast specimens appeared to be a typical hypoeutectic structure. From the results of the backscattered electron image (BEI) and energy dispersive spectrometry (EDS), the difference between the composition of the α-Mg and Ni-rich eutectic regions was distinguished clearly. The hydrogenation properties of Mg-Ni alloys depended on the behavior of the nickel compositions. Especially, the hydrogen kinetics of Mg-9 mass%Ni was more excellent than the others.