The hydrogen storage properties of Zr1-xCrxFe2 (x = 0.2, 0.3, 0.4, 0.5) alloys have been obtained in the pressure and temperature range of 0.5 <= P <= 60 bar and 303 K <= T <= 373 K. The alloys have been characterized by XRD and SEM. The results show that all the alloys were having C14 laves phase hexagonal structure. The substitution of Cr in Zr site leads to the contraction of their lattice. The P-C-T isotherms of the alloys showed the existence of alpha, alpha + beta, and beta regions. The maximum hydrogen intake capacity is around 3.131 H/f.u. at 303 K and at 48 bar pressure for Zr0.8Cr0.2Fe2 alloy. The average relative partial molar enthalpy and entropy of hydrogen at plateau region have been calculated for all the alloys. The presence of alpha, alpha + beta, and beta region as seen in P-C isotherm has been confirmed by the variation of thermodynamical parameters with hydrogen content. (C) 2007 International Association for Hydrogen Energy. Published by Elsevier Ltd. All rights reserved.