The aim of this study is to understand the remarkable improvements achieved on the hydrogenation properties of TiFe alloy modified by Zr7Ni10 alloy. For this purpose, comparative effect of 4 wt% Zr, Ni and Zr7Ni10 alloy addition on hydrogenation, morphological and structural properties of TiFe alloy were investigated. Our results show that while zirconium addition has positive influence on hydrogen absorption capacity and kinetics of TiFe alloy, nickel addition has negative effect on these properties. Specific microstructure and Fe/Ti atomic ratio in intergranular phases are responsible for the obtained results. More specifically the present study shows that by zirconium addition, TiFe alloy could absorb hydrogen under moderate temperature-pressure conditions without any prior treatment. This modified system is also resistant to air exposure. Copyright (C) 2015, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights reserved.