In order to improve the hydrogenation property of Mg/Ti laminate composite, Ni was added as a third element. Hydrogen storage properties of the laminated Mg/Ti/Ni alloy films were studied. Laminated Mg/Ti/Ni multilayer alloy films were prepared by cold rolling of stacked Mg, Ti and Ni under ambient conditions. The stacked foils were subjected to repetition of rolling and stacking, resulting in super-laminated foils with the thickness less than 0.3mm, containing more than 15000 layers. Microstructures of the super-laminates were studied by scanning electron microscopy and X-ray diffractometry. Their hydrogenation behaviors were investigated by use of a Sieverts type apparatus. The hydrogen storage capacity (H/M) of the laminate with composition Mg/Ti/Ni=9.0/0.9/0.1 amounted H/M=1.6 at 573K, 0.4MPa. Initial activation property was improved by controlling the amount of Ni appropreately.