Ball-milled nanocrystalline Mg2Ni powders were subjected to intense plastic straining by cold rolling or equal-channel angular pressing. Morphological and microstructural evolution during these processes has been investigated by scanning electron-microscopy and Xray diffraction line profile analysis, respectively. Complementary hydrogen absorption experiments in a Sieverts' type apparatus revealed that there exists some correlation between the micro- and nanostructure and hydrogen storage properties of the severely deformed materials. Copyright (C) 2014, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights reserved.