It is still a challenge to achieve simultaneous improvements in aging resistance, mechanical strength, thermal conductivity and dielectric constant of rubber composites via incorporation of graphene obtained by conventional methods. Herein, an effective and green method was proposed to simultaneously reduce and functionalize graphene oxide (GO) with 2-mercaptobenzimidazole (antioxidant MB) via a one-pot method. GO was successfully reduced by MB which was also chemically grafted on the reduced GO (G-MB). G-MB sheets were uniformly dispersed in rubber with strong interfacial interaction, and graphene-graphene conductive paths were formed through intermolecular H-bonding between the grafted antioxidant molecules. Consequently, rubber composites with G-MB showed higher thermal conductivity, mechanical strength and dielectric constant than rubber composites with hydrazine hydrate reduced GO (rGO). Moreover, the thermo-oxidative aging resistance of rubber composites with G-MB was also superior to that of rubber composites with rGO because of the elimination of blooming effect of the grafted MB molecules. Thus, this work may open a new way for the eco-friendly functionalization and reduction of GO and may boost the development of high-performance, functional graphene-elastomer composites. (C) 2019 Elsevier Inc. All rights reserved.