The thermomechanical and tribological properties of graphene (GNS)-reinforced NR were investigated using molecular dynamics (MD) simulations. The amorphous molecular dynamics models of two nanocomposites, i.e., natural rubber (pure NR) and graphene/natural rubber (GNS/NR), were established. In addition, the thermodynamic properties of the two materials, before and after the incorporation of graphene into the natural rubber matrix, were investigated through analytical comparison. The results showed that after the graphene was added to the rubber matrix as a reinforcing material, the elastic modulus and shear modulus were increased by 110% and 94.8%, respectively, the tensile property was increased by 178%, the overall thermal conductivity of the composite system was increased by 59%, the glass transition temperature increased from 223 K to 236 K, and the rigidity of the material matrix was significantly improved. The inherent interactions and wear mechanisms of the polymer nanocomposites were discussed at the atomic scale by analyzing the changes in temperature, atomic velocity, relative atomic concentration, and radial distribution functions at the friction interface in the thickness direction.

Based on the electronic universal testing machine with a temperature chamber, this paper investigated the temperature and filler effects on the hyper-elastic behavior of reinforced rubbers and revealed the regulation of the stress and strain of the natural rubber and filled rubber with temperature. The experimental results showed that the hyper-elastic behavior of the filled rubber was temperature-dependent in a wide range. Comparing the adaptability of different models to the stress–strain variation with temperature, the Yeoh model was proven to reasonably characterize the experimental data at different temperatures. Based on the Yeoh model, an explicit temperature-dependent constitutive model was developed to describe the stress–strain response of the filled rubber in a relatively large temperature range. The prediction data of this proposed constitutive model fit well with the test data of the mechanical experiments, indicating that the model is suitable to characterize the large deformation behavior of filled rubbers at different temperatures to a certain degree. The proposed model can be used to obtain the material parameters and has been successfully applied to finite element analysis (FEA), suggesting a high application value. Notably, the model has a simple form and can be conveniently applied in related performance tests of actual production or finite element analysis.