The effect of carbon nanomaterials (ultradispersed diamond–graphite blends, and ultradispersed diamonds) on the microplasma oxidation of aluminum alloys is studied. It is shown that the introduction of carbon nanomaterials into the electrolyte leads to the intensification of the coating formation process. This is evident from the increase in the coating’s thickness by a factor of 1.8–2.5 depending on the chemical composition of the alloys. A more significant effect is found for diamond–graphite blends. The surface modification with particles of nanodiamond and nanographite leads to an increase in the microhardness, wear resistance, and bearing capacity and to a decrease in the friction coefficient.