The precursors of hydrotalcite-like structures of Ni-Cu-Al catalysts derived with different Cu/Al ratios have been synthesized by coprecipitation method. The CH4 decomposition activities are evaluated at 600-700 degrees C and ambient pressures over calcined Ni-Cu-Al catalysts until the catalysts were deactivated completely. The physico-chemical characteristics of the fresh catalysts are obtained using BET surface area, X-ray diffraction (XRD), temperature programmed reduction (TPR), TGA, SEM/EDAX and X-ray photoelectron spectra (XPS) analyses and the deactivated catalysts are investigated by transmission electron microscopy (TEM), Raman and CHNS analyses. The Raman spectra revealed the presence of both ordered and disordered forms of carbon in the deactivated catalysts. Higher H-2 yields are obtained over Ni-Cu-Al (60:25: 15 mol%) catalyst. (c) 2008 Published by Elsevier Ltd. on behalf of International Association for Hydrogen Energy.