Mg - 40 wt % TiFe nanocomposite was prepared by high-energy ball milling, HEBM, aiming improved hydrogen absorption at room temperature (RT). Four processing routes were chosen to separately investigate the effects of TiFe addition, HEBM processing and dispersion of TiFe particles, being: Route 1 - mechanical mixture of Mg and TiFe powders; Route 2 - HEBM of Mg + TiFe at 400 rpm for 12 h; Route 3 - HEBM of pure Mg at 400 rpm for 12 h to be used as reference; and Route 4 - HEBM of Mg + TiFe at 600 rpm for 36 h. In this case, TiFe was previously milled with ethanol to improve its refinement level. It is shown that the synergetic effects of TiFe addition, HEBM processing and thermal activation - involving the creation of Mg-TiFe interfaces, the refinement and distribution of TiFe and also the presence of free Fe - lead to good hydrogenation kinetics at RT in Mg-TiFe nanocomposite. It is also shown for the first time that the milled pure Mg can absorb hydrogen at RT. (C) 2018 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.