In recent years, composites have been widely used in engineering fields, where nanomaterials such as graphene (Gr) and graphene oxide (GO) have potential advantages as interfacial modifiers in enhancing the properties of composites. However, the relationship between the interfacial structure and the mechanical properties of the nanocomposites is not clear, and the behavior of the composites may differ significantly at different temperatures. This study aims to investigate in depth the interfacial structure, dynamics, and mechanical properties of Gr, epoxy group-containing (-O) and hydroxyl group-containing (-OH) graphene oxide and calcium aluminosilicate hydrate (C-A-S-H) composites at different temperatures using molecular dynamics. The effect of nanomaterial composition on the interfacial chemical bonding network is revealed. The local chemical structures of bridging aluminum [Al(Q2b)] and interlayer aluminum (Alw) show different changes at different temperatures. Elevated temperature promotes the hydrolysis of interlayer water molecules to form hydroxyl groups, which affects the formation of chemical bonding networks.Al(Q2b) favors Gr and C-A-S-H linkages, whereas Alw favors GO and C-A-S-H bonding. Temperature changes lead to different chemical bonding connections and altered atomic motions. At the interface, Al atoms form a more stable chemical bonding network, which improves the interaction strength at the interface. Different composite models exhibited different mechanical properties at high temperatures and introducing epoxy and hydroxyl groups enhanced the plastic deformation of the composites. Structural analyses showed that temperature changes affected the molecular structure and interfacial bonding effects of the composites, which in turn affected the mechanical properties of the materials. At different temperatures, GO-O/C-A-S-H has higher tensile strength and Young's modulus, which can resist the degradation of performance caused by thermal expansion to a certain extent, and ensure the stability and safety of the structure, so it is more practical. These findings provide important insights to deepen the understanding of composite properties and have positive implications for future composite design and applications.