The catalytic production of hydrogen by steam reforming of methanol (SRM) has been carried out over Mg/Al, Cu/Al, Co/Al, and Ni/Al layered double hydroxides (LDHs), The catalytic reactions were performed at temperatures of 150-400degreesC and atmospheric pressure. The most efficient catalyst was the Cu/Al LDH, which became active at similar to230 degreesC, with concomitant H-2 production. The Ni/Al and Co/Al LDHs were also active in SRM however, the activation temperature was significantly higher (315-320 degreesC). No catalytic activity was observed for the Mg/Al LDH. Significant LDH decomposition occurred during the catalytic reactions. The reducibility of the divalent cations present in the LDH was a crucial parameter in determining 9 the steam reforming activity of the catalysts, Pre-activation of the Cu/Al LDH by calcination in air (400 degreesC), followed by reduction in dilute H-2 did not significantly change the catalytic activity. The onset of H-2 production was slightly lower for the pre-activated versus as-prepared Cu/Al LDH (similar to218 degreesC), also the CH3OH conversion was 5 - 10% lower.