The Mechanically Activated Self-propagating High temperature Synthesis (MASHS) has been employed to obtain nanostructured Mg2Ni alloys. MASHS process has been further improved by controlling the electrical parameter measurements during the combustion reaction under the thermal explosion mode. The samples were hydrogenated at 20 bar and 300 degrees C by means of a Pressflow Gas Controller while the dehydrogenation was conducted in a Differential Scanning Calorimetry (DSC) equipped with an H-2 detector of the purged gas. Nanostructured Mg2Ni demonstrated hydrogen storage capacity around 3.5 wt%. The desorption temperature was about 250 degrees C at 3 degrees C/min. The activation energy for dehydrogenation, calculated by the Kissinger method, was about 100 kJ/mol. Copyright 2011, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights reserved.