Graphite is a well-known solid lubricant and can be as important as clay minerals in reducing the frictional strength of faults. Some natural fault zones contain carbonaceous material (CM) even where host rocks do not contain it, and seismic fault motion can promote the graphitization of low-grade CM. Thus, the origin of CM in fault zones is an important issue in fault mechanics. Previous high-velocity friction experiments have revealed various chemical reactions in fault zones during seismic fault motion, but most experiments have been conducted in an atmosphere under oxic conditions. Here we report experimental results on Carrara marble (free of CM), conducted under N2 or H2 atmospheres at a slip rate of 1.3 m/s and normal stresses of 2.0–3.1 MPa. A small amount of blackish material formed in generated gouge only under reducing conditions with the H2 atmosphere, and Raman spectroscopic analysis revealed the presence of CM (amorphous carbon) in the material. The CM is attributable to (1) the generation and pyrolitic dissociation of CH4, and/or (2) a reduction reaction of emitted CO2 due to calcite decomposition. We confirmed the formation of CH4 using gas chromatography. The CM produced in experiments resembles CM in the Nojima fault (Japan) gouge in terms of Raman spectra. The granitic host rock of this fault is free of CM, and calcite is precipitated close to the CM; therefore, the CM probably formed through processes similar to those simulated in our experiments. Future research should investigate the amount and origin of CM in natural fault zones.