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Nanoindentation tests and molecular dynamics (MD) simulations are conducted to investigate the effect of graphene (Gr) coating on the deformation behavior of a <001> orientation copper (Cu) substrate. Distinct displacement burst (pop-in) is observed in the load-depth curve, which is due to the fracture of the Gr coating. Compared to bare Cu, the MD simulations indicate different dislocation activities at the Gr/Cu interface. The effect of image stress confinement on the glide of dislocations in Cu is considered to be the reason responsible for the increased hardness in the Gr/Cu system.