The thermodynamic properties of CeMn1-xAl1-xNi2x (x = 0.00, 0.25, 0.50 and 0.75) hydrides have been investigated in this paper, With increasing Ni substitution content, the hydrogen concentration (H/M) in CeMn1-xAl1-xNi2x (x = 0.00, 0.25, 0.50 and 0.75) hydride increases from 0.129 wt% for x = 0.00 to 0.421 wt% for x 0.75 at 293 K. The pressure-concentration isotherm (P-C-T) curves show that no hydrogen equilibrium pressure plateau has been observed for CeMnAl hydride while the slope of the plateau become flatter and longer with increasing Ni content. Meanwhile, the enthalpy change (Delta H-0) and the entropy change (Delta S-0) of the hydrides for dehydrogenization shift from -67.44 kJ mol(-1) (x = 0.00) to 21.16 kJ mol(-1) (x = 0.75) and from -0.24kJ mol(-1) K-1 (x = 0) to -0.03 kJ mol(-1) K-1 (x = 0.75), respectively. With increasing Ni content, both Delta H-0 and Delta S-0 for dehydrogenization shift to the positive direction and make alloy hydrides more stable and hydrogen desorption much easier. (C) 2008 International Association for Hydrogen Energy. Published by Elsevier Ltd. All rights reserved.