A non-equilibrium deformation simulation based on standard molecular dynamics is employed to reveal the physical origin of distinct mechanical properties of polymer nanocomposites (PNCs) reinforced by polymer tethered graphene nanosheets (P/G-T). The effect of tethered polymer length (L) and interaction strength on the mechanical properties, including tensile stress, modulus, and yield strength, are examined. The simulation results show that the P/G-T systems exhibit improved mechanical properties as L and interaction strength increases. The strengthening in attractive interaction between matrix polymer and tethered polymer has a better effect on mechanical properties than that between P and graphene nanosheets. It is found that the bond orientation and nonbonding potential is of crucial importance in determining the mechanical properties of the P/G-T nanocomposite systems. The calculations of radial distribution functions and mean-squared displacement are further performed to reveal the physical origin of enhanced mechanical properties, suggesting that the stronger interfacial interactions will induce the closer packing distance with smaller free volume, higher polymer chain entanglement, and higher restriction of polymer chain movement, which synergistically contribute to the improvement in the mechanical properties. The results may provide useful guidance for promoting the development and practical application of the advanced PNCs with excellent performance.