This study proposed the new method of preparing Mg-based composite by mixed powder Ni and Ti onto the surface of pure Mg ingot. The prepared method caused that hydrogen absorbing phase Mg2Ni and catalytic phase NiTi generated and distributed regularly. The pure Mg ingot as the center and the powder Ni and Ti as cladding material on the surface were formed and sintered, in which the temperature range of generated alloy phase Mg2Ni and NiTi was confirmed at first; according to the temperature range, the size of Mg2Ni and NiTi crystal grains at 650°C and 850°C were analyzed and compared, respectively; The size of Mg2Ni alloy phase at the surface and center was calculated by comparing the atomic radius of Ni, Ti to confirm that Mg2Ni distributed on the surface due to the atom Ti replaced the atom Ni in Mg2Ni to generate the alloy phase NiTi; the capacity of the hydrogen desorption reached 4wt% within 5min. The disadvantages that easy to chalking and difficult to activate in the conventional method were avoided and achieved the application of the multilayer composite material in hydrogen storage field.