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In the present work, we investigate the wear mechanisms of a Cu bi-crystal containing a random high angle grain boundary by means of molecular dynamics simulations. The underlying deformation behavior of the material is analyzed and further related to the observed characteristics of mechanical response and resulting morphology of the worn surface. In particular, the grain boundary-associated mechanisms are characterized by advanced analysis techniques for lattice defects. Our simulation results indicate that in addition to dislocation slip and dislocation-grain boundary interactions, grain boundary migration plays an important role in the plastic deformation of Cu bi-crystal. It is found that the wear behavior of Cu depends on the crystallographic orientation of the worn surface and can be altered quite significantly by the presence of a grain boundary.