Hydrogenation properties of pseudo-binary Ti1.02-xZrxNi0.98 (0 <= x <= 0.48) intermetallic compounds have been investigated. The substitution of Zr for Ti in TiNi compound leads to a high increase of the storage capacity both in solid-gas reaction (1.4 hydrogen atoms per formula unit, H f.u.(-1) for TiNi and 2.6 H f.u.(-1) for the substituted compounds) and electrochemical reaction (150 mAhg(-1) for TiNi and similar to 350mAhg(-1) for the substituted compounds). The high capacity of the substituted compounds is closely linked to the martensitic transformation that occurs in TiNi-type intermetallic compounds. (C) 2008 International Association for Hydrogen Energy. Published by Elsevier Ltd. All rights reserved.