The Zr(V1-xFex)(2) (x=0.02, 0.05, 0.10, 0.15, 0.25) alloys were prepared by the arc-melt method and annealed at 1273 K for 168 h in an argon atmosphere. Phase structure investigations of the as-cast and annealed Zr(V1-xFex)(2) alloys indicate the annealing treatment can eliminate the minority phases originating from the non-equilibrium solidification of as-cast alloys. The ZrV2-type phase becomes the dominant one in each annealed alloy. The substitution of Fe in V sites leads to the contraction of their lattice. For annealed Zr(V1-xFex)(2) alloys, the P-t and PCT curves obtained between 673 K and 823 K give the evidence that the absorption process is controlled by a rate-controlling hydrogen diffusion. With the increase of iron, the equilibrium pressure and the plateau slope increase while the hydrogenation capacity and the absolute value of enthalpy and entropy decrease accordingly. The stability of metal hydride reduces gradually as the Fe content varies from x = 0.02 to 0.25 which promotes the hydrogen release and favors the practical applications of the Zr(V1-xFex)(2) alloys. Copyright (C) 2011, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights reserved.