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Tribological shearing of polycrystalline metals typically leads to grain refinement at the sliding interface. This study, however, shows that nanocrystalline metals exhibit qualitatively different behavior. Using large-scale atomistic simulations, we demonstrate that during sliding, contact interface nanocrystalline grains self-organize through extensive grain coarsening and lattice rotation until the optimal plastic slip orientation is established. Subsequently, plastic deformation is frequently confined to localized nanoshear bands aligned with the shearing direction and emanating from voids and other defects in the vicinity of the sliding interface.