A hybrid graphene/Ni2+–Fe3+ layered double hydroxide material has been fabricated by the hydrothermal treatment of a mixed suspension of the exfoliated graphite oxide, Ni(NO3)2 6H2O, Fe(NO3)3·9H2O, urea and trisodium citrate. The Ni2+–Fe3+ layered double hydroxide platelets are first homogeneously grown on the surface of GO nanosheets which are then reduced to graphene under a mild hydrothermal treatment. In the hybrid graphene/Ni2+–Fe3+ layered double hydroxide material, the restacking of graphene nanosheets is effectively prevented by the formation of Ni2+–Fe3+ layered double hydroxide platelets, and the graphene nanosheets exist in a complete exfoliation state.