The debonding behavior of graphene/graphene oxide on calcium silicate hydrate substrate directly affects the performance of gelling composites, however it is difficult to achieve the debonding effect in traditional experiments. In order to clarify the debonding characteristics of graphene/graphene oxide, the debonding behavior of graphene/graphene oxide on calcium silicate hydrate substrate at nanoscale by molecular dynamics method was studied. The results show that the bonding properties of graphene/graphene oxide decrease with the increase of temperature, compared with graphene, the change of temperature has a greater effect on the bonding properties of graphene oxide. Among graphene oxide, epoxy-based graphene oxide is least affected by the change of temperature. The main factors affecting the bonding properties are the van der Waals forces and Coulomb interactions between graphene/graphene oxide and calcium silicate hydrate. High concentration and functional groups at the edge can significantly enhance bonding properties, and the effect of different functional groups on enhancing bonding properties is carboxyl group, hydroxyl group and epoxy group.