Pull-out processes were simulated to investigate the interfacial mechanical properties between the functionalized graphene sheet (FGS) and polyethylene (PE) matrix by using molecular dynamics simulation with ReaxFF reactive force field. The interfacial structure of polymer and the interfacial interaction in the equilibrium FGS/PE systems were also analyzed to reveal the enhancement mechanism of interfacial shear strength. We observed the insertion of functional groups into polymer layer in the equilibrium FGS/PE systems. During the pull-out process, some interfacial chains were attached on the FGS and pulled out from the polymer matrix. The behavior of these pulled out chains was further analyzed to clarify the different traction action of functional groups applied on them. The results show that the traction effect of functional groups on the pulled-out chains is agreement with their enhancement influence on the interfacial shear strength of the FGS/PE systems. They both are basically dominated by the size of functional groups, suggesting the enhancement mechanism of mechanical interlocking. However, interfacial binding strength also exhibits an obvious influence on the interfacial shear properties of the hybrid system. Our simulation show that geometric constrains at the interface is the principal contributor to the enhancement of interfacial shear strength in the FGS/PE systems, which could be further strengthened by the wrinkled morphology of graphene in experiments. (C) 2016 Elsevier B.V. All rights reserved.