In this paper, we describe and discuss the synthesis, structural-microstructural and hydrogen storage behaviour of three AB(2) type storage materials namely (a) ZrFe2 (b) Zr(Fe(0.7)5V(0.25))(2) and (c) Zr(Fe0.5V0.5)(2). These alloys were synthesied by radio frequency induction melting in argon atmosphere. X-ray diffraction and transmission electron microscope have been employed for structural and microstructural characterizations. The XRD study reveals that the lattice constants and the unit cell volume of ZrFe2, Zr (Fe0.75V0.25)(2), Zr(Fe0.5V0.5)(2) alloys, which has C14 type hexagonal Laves phase. The Surface morphology and elemental composition of these alloys were investigated by scanning electron microscope and energy dispersive X-ray analysis. The pressure composition isotherms of these alloys were investigated at room temperature and pressure ranges of 0-100 atm respectively, measured through a fully computerized PCI apparatus. As we increase the concentration of V (substituted for Fe), the total hydrogen storage capacities increased up to 1.45 wt%. This capacity is achieved in Zr(Fe0.5V0.5)(2) alloy, while the reversible hydrogen storage capacity decreases due to the formation of a stable hydride phase. It has been found that the lattice constants increase with higher vanadium concentration. This is indicating that the majority of vanadium atoms reside in the B-site. The broader X-ray diffraction peaks observed in Zr(Fe0.5V0.5)(2) alloy indicates a higher degree of disorder for alloys with the higher V-content. The yet another interesting feature observed in our present study is that the plateau pressure remains well below 1 atm for all the compositions. Copyright (C) 2011, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights reserved.