Graphene decorated with Fe clusters is proposed to be a possible alternative catalyst for the hydrogenation and dehydrogenation reactions of MgH . In particular, graphene decorated with Fe clusters is effective for both hydrogenation and dehydrogenation processes of MgH . The change in enthalpy and entropy values of hydrogen absorption determined for MgH with 5 wt% graphene decorated with Fe clusters is −50.4 ± 2.9 kJ per mole of H and 99.8 ± 5.2 J K per mole of H , respectively.