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The influence of the surface mechanical-pulse treatment based on high-speed friction with a rapid cooling by the technological environment on the wear resistance of medium- and high-carbon steels was considered. The treatment due to a severe plastic deformation enabled obtaining the nanocrystalline structure with a grain size of 14–40 nm. A high positive effect of this treatment was obtained not only because of metal nanocrystallization but also thanks to other factors, namely, structural-phase transformations, carbon saturation of the surface due to decomposition of the coolant and the friction coefficient decrease. Higher carbon content leads to better strengthening of the surface, and its microhardness can reach 12 GPa.