This investigation was conducted to evaluate the effect of cold rolling on the structure and hydrogen properties of two magnesium alloys, AZ91 and AM60D, after processing by equal-channel angular pressing (ECAP). The results show that the use of cold rolling after ECAP significantly increases the preferential texture for hydrogenation and increases the potential for the use of these alloys as hydrogen storage materials. The ECAP was performed through two different numbers of passes in order to give different grain sizes and both materials were subsequently cold-rolled through the same numbers of passes for a comparison of the hydrogenation absorption. It is shown that the hydriding properties are enhanced by an (0001) texture which improves the kinetics primarily in the initial stages of hydrogenation. The results demonstrate that optimum sorption properties may be acquired through a combination of fine grains and appropriate texture.