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The nature of nanocrystalline materials determines that their deformation at the grain level relies on the orientation of individual grains. In this work, we investigate the anisotropic response of nanotwinned Cu to frictional contacts during nanoscratching by means of molecular dynamics simulations. Nanotwinned Cu samples containing embedded twin boundaries parallel, inclined and perpendicular to scratching surfaces are adopted to address the effects of crystallographic orientation and inclination angle of aligned twin boundaries cutting the scratching surface. The transition in deformation mechanisms, the evolution of friction coefficients and the friction-induced microstructural changes are analyzed in detail and are related to the loading conditions and the twinned microstructures of the materials. Furthermore, the effect of twin spacing on the frictional behavior of Cu samples is studied. Our simulation results show that the crystallographic orientation strongly influences the frictional response in different ways for samples with different twin spacing, because the dominant deformation mode varies upon scratching regions of different orientations. A critical inclination angle of 26.6° gives the lowest yield strength and the highest friction coefficient, at which the plasticity is dominated by twin boundary migration and detwinning. It is demonstrated that the anisotropic frictional response of nanotwinned Cu originates from the heterogeneous localized deformation, which is strongly influenced by crystallographic orientation, twin boundary orientation and loading condition.