Two processes for production of synthesis gas and pure hydrogen from methane using chemical looping were investigated using CuO-Fe2O3-alumina oxygen carriers. In the first process, CuO-Fe2O3 was initially reduced with methane and the reduced oxygen carrier was used as a catalyst for decomposition of methane to produce hydrogen; then the carbon formed during the methane decomposition was gasified with steam to produce synthesis gas. Methane chemical looping combustion with CuO-Fe2O3 oxygen carrier provides the heat for both the methane decomposition and carbon gasification reaction. In the second process, the reduced Cu-Fe oxygen carrier was used as a methane steam reforming catalyst to produce synthesis gas from steam and methane. Heat for the reforming reaction is provided by the methane chemical looping combustion reaction of the Cu-Fe oxygen carrier. Multiple-cycle tests of those process steps have been experimentally evaluated in a bench-scale flow reactor. Both processes use the same CuO-Fe2O3 oxide system, as an oxygen carrier for chemical looping combustion reactions and as a catalyst for methane decomposition and methane steam reforming reactions. Copyright (C) 2014, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights reserved.