The CO2 reforming of methane over an alumina-supported nickel catalyst has been studied using a conventional micro-reactor set-up. These experiments have been used to guide inelastic neutron scattering (INS) measurements, which were performed post-reaction using a ‘quench’ technique. The reacted catalyst has also been examined using infrared spectroscopy and transmission electron microscopy. This unified approach reveals the presence of a hydrogen-lean coke to have formed during the reforming process, which is predominantly comprised of amorphous carbon, the domains of which appear to be terminated with a small number of hydrocarbon groupings. A semi-quantitative analysis of the INS spectra establishes the catalyst to be very effective in cycling hydrogen during the reforming process.