In the development of metal hydrides for commercial applications, a special attention should be devoted to the ways of production. For commercial success, the raw elements of the hydrogen storage materials should be of low cost, the synthesis process should be inexpensive and easily scalable. Therefore, it is important to put some effort on the elaboration of new and more efficient means of producing metal hydrides. In this perspective, cold rolling was investigated as a new means of producing nanocrystalline materials. This technique is well-known in the industry and easily scalable. Cold rolling was performed on Mg-Ni system. The evolution of morphology, crystal structure, crystallite size, deformation, and preferred orientation was studied as a function of number of rolling passes. Cold rolling followed by a heat treatment produced the intermetallic Mg2Ni. Without heat treatment and for a large number of rolling, an amorphous phase was synthesized.