The brush materials modified with organosilicon were prepared by the powder metallurgy method, and their current-carrying friction and wear properties were compared with those of brush materials modified with SiO2. The materials were characterized by SEM, XRD, XPS, deep etching, and roughness. The results showed that, compared with the SiO2, organosilicon can significantly reduce the wear rate of brush materials by 67–88%, because the SiOC fiber produced by pyrolysis of organosilicon could control the graphite content on the friction surface by reducing abrasive wear. In the aspect of wear mechanism, organosilicon could greatly reduce the abrasive wear of the materials and the mated materials, but aggravated the adhesive wear of the materials.