Magnesium (Mg) is a light metal with relatively low cost. Its hydride (MgH 2 ) is interesting for the safe hydrogen storage in solid state and has a high gravimetric capacity of 7.6%. Practical application of Mg is still hampered by high reaction temperatures and slow kinetics. In order to improve it and focus on more viable industrial processing conditions, Mg plates, with or without iron (Fe) addition, in the form of wires and powders, were submitted to severe plastic deformation (SPD) in air, starting with extensive cold rolling (ECR), followed by repetitive rolling (ARB). The samples were characterized by X-ray diffraction (XRD), optical microscopy (OM), scanning (SEM) and transmission electron microscopy (TEM). H 2 storage properties were evaluated by differential scanning calorimetry (DSC) and Sievert's volumetric method. Mg processed by ECR+ARB resulted in larger grain refinement and densities of cracks than ECR. In addition, Fe in the form of continuous wires was fragmented and resulted in a better distribution of particles than powders, which agglomerated. Thus, finally, the synergetic effect of microstructural features and Fe as catalyst and its distribution improved activation, kinetics and hydrogen storage capacity.