Pure hydrogen was obtained by catalytic methane decomposition over thermally stable nickel-based catalysts prepared from hydrotalcite-like precursors. Two different Ni-Mg-Al catalyst compositions were tested in the catalytic pyrolysis reaction of methane. The catalytic results were compared with those of a catalyst prepared by conventional impregnation of Ni-Mg phases on an alumina support. The high thermal stability of these catalysts was demonstrated in several reaction-regeneration cycles. The regeneration processes were performed with CO2 and O-2 as regenerating agents. Using either CO2 or O-2 gas, hydrogen production after regeneration increased with regard to the fresh catalyst. Upon catalyst regeneration, larger amounts of hydrogen were obtained on catalysts regenerated with CO2 than with O-2. The high thermal stability of the Ni particles of the catalysts from hydrotalcite-like precursors was improved in the presence of Mg. This high Ni-stability is a key factor for increasing hydrogen production after consecutive reaction-regeneration cycles. (C) 2006 Elsevier B.V. All rights reserved.