In the present work, we have processed 2Mg-Fe mixtures by reactive milling (RM) under hydrogen atmosphere to synthesize Mg2FeH6 phase in the powder form which were then systematically processed by High Pressure Torsion (HPT) to produce bulk samples. The bulk samples were characterized in terms of microstructural and structural analyses and of hydrogen desorption properties. The hydrogen sorption properties after HPT processing was evaluated in comparison with the Mg2FeH6 powder obtained by RM and with commercial MgH2. HPT processing of Mg2FeH6 can produce bulks with a high density of defects that drastically lower the activation barrier for hydrogen desorption. Therefore, the bulk nanocrystalline Mg2FeH6 samples show endothermic hydrogen decomposition peak at a temperature around 320°C. In addition, when compared with the Mg2FeH6 and MgH2 powders, the Mg2FeH6 HPT disks showed the same results presented by the Mg2FeH6 powders and certainly decreases the onset transition temperature by as much as 160°C when compared with the MgH2 powders.