In this paper we report the role of morphology and severe plastic deformation on the hydrogen storage properties of magnesium. Samples were prepared in air at room temperature by accumulative roll-bonding, filing and a combination of both processes. Accumulative roll-bonding drastically refined the microstructure of magnesium but resulted in a limited hydrogen capacity. Filing accelerated the activation of magnesium without compromising hydrogen capacity. Combining both techniques enhanced or worsened the hydrogen storage properties depending on the processing sequence. These results are explained in terms of microstructure and morphology of the samples. Copyright (C) 2014, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights reserved.