Ball-milled nanocrystalline Mg 2 Ni 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 X-ray 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.