Synergistic effect of metallic couple and carbon nanotubes on Mg results in an ultrafast kineticsof hydrogenation that overcome a critical barrier of practical use of Mg as hydrogen storage materials. Theultrafast kinetics is attributed to the metal-H atomic interaction at the Mg surface and in the bulk (energyfor bonding and releasing) and atomic hydrogen diffusion along the grain boundaries (aggregation of carbonnanotubes) and inside the grains. Hence, a hydrogenation mechanism is presented.