Catalysts with high nickel concentrations 75%Ni-12%Cu/Al2O3, 70%Ni-10%Cu-10%Fe/Al2O3 were prepared by mechanochemical activation and their catalytic properties were studied in methane decomposition. It was shown that modification of the 75%Ni-12%Cu/Al2O3 catalyst with iron made it possible to increase optimal operating temperatures to 700-750 degrees C while maintaining excellent catalyst stability. The formation of finely dispersed Ni-Cu-Fe alloy particles makes the catalysts stable and capable of operating at 700-750 degrees C in methane decomposition to hydrogen and carbon nanofibers. The yield of carbon nanofibers on the modified 70%Ni-10%Cu-10%Fe/Al2O3 catalyst at 700-750 degrees C was 150-160 g/g. The developed hydrogen production method is also efficient when natural gas is used as the feedstock. An installation with a rotating reactor was developed for production of hydrogen and carbon nanofibers from natural gas. It was shown that the 70%Ni-10%Cu-10%Fe/Al2O3 catalyst could operate in this installation for a prolonged period of time. The hydrogen concentration at the reactor outlet exceeded 70 mol%. (C) 2009 International Association for Hydrogen Energy. Published by Elsevier Ltd. All rights reserved.