A first investigation into the production of amorphous and nanostructured Ti-based alloys with nominal compositions Ti41.5Zr41.5Ni17, Ti61Zr22Ni17, Ti41.5V41.5Ni17 and Ti61V22Ni17 by mechanical alloying (MA) technique is presented. This technique was adopted to produce alloys powders with high fresh surface area that were active for hydrogen storage. Hydrogen absorption characteristics and structure changes in the alloys after hydrogenation were investigated. Gas phase hydrogenation of the Ti-Zr-Ni alloys, at 573 K and an initial hydrogen pressure of 2 MPa, exhibited good hydriding properties and started at a maximal rate without induction period with a hydrogenation capacity up to 1.2 wt%. However, hydriding of Ti-V-Ni alloys at the same conditions exhibited slower rates. The Ti61V22Ni17 composition showed high hydrogen absorption capacity of 1.8 wt% and exceeded 4 wt% at 345 K. In addition, the Ti-V-Ni alloys showed structure stability after hydrogenation and retained the amorphous structure. Copyright (C) 2014, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights reserved.