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The role of graphite/substrate interface in low-friction behavior of graphite was investigated. Iron and graphite powder mixtures were plastically deformed in either Ar–H2 or air atmospheres to obtain bare iron or iron oxide surface. Then, graphite particles adhered to and formed interfaces with surfaces. Friction force microscopy revealed that friction on particle surface milled in Ar–H2 atmosphere was obviously higher. X-ray absorption near-edge structure and transmission electron microscopy revealed that although the basal plane of graphite oriented along the oxidized surface, it did not occur along the bare iron surface, which explains the difference in lubricity on each surface.