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In this study, commercial AZ31 Mg alloys were processed by equal channel angular pressing (ECAP) to study the effects of processing route and numbers of passes on hydrogen storage properties of AZ31 alloys. Furthermore, Mg-based metal matrix composites (MMCs) were fabricated by gravimetric casting of AZ31 alloy, activated carbon and Ni to investigate the effect of additives on hydrogen storage properties. The results indicated that kinetics of hydrogen uptake increased with the increasing number of pass. AZ31 processed by ECAP route B c with 8 passes had hydrogen capacity of 7.0 wt%, and demonstrated the highest grain refinement and the fastest hydrogen absorption kinetics. With the addition of 5 wt% of activated carbon and 0.5 wt% Ni, the hydrogen sorption kinetics of MMCs was enhanced and was comparable to that of the AZ31 processed by ECAP with 8 passes; however, in exchange for the improved kinetics, the hydrogen storage capacity was lowered to 6.3 wt%. To enhance hydrogen absorption kinetics, adding catalysts in the casting process could be more efficient than post-casting ECAP treatment if saving processing time is the priority. [ABSTRACT FROM AUTHOR]