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The service life of artificial joints has gradually failed to meet the needs of patients. Herein, the synergistic lubrication and antioxidant efficacies of graphene oxide (GO) and fullerenol (Fol) as biological lubricant additives for artificial joints were investigated. The lubrication mechanisms of biological lubricant containing GO and Fol at the friction interface of artificial joints were then revealed. Tribological tests showed that the average friction coefficients of Al2O3–Ti6Al4V pairs and Ti6Al4V–UHMWPE pairs for artificial joints could be reduced by 30% and 22%, respectively, when GO and Fol were used as biological lubricant additives simultaneously. The lubrication mechanism showed that some incommensurate sliding contact surfaces could be formed between the GO nanosheets and spherical Fol at the interface, which reduced the interaction forces of friction pairs. The maximum scavenging rates of •OH and DPPH free radicals by the biological lubricant containing GO and Fol were 35% and 45%, respectively, showing a good antioxidant efficacy of the biological lubricant. This can be attributed to the GO and Fol scavenging free radicals through electron transfer and hydrogen transfer. This study provides a theoretical basis for the development and application of carbon nanomaterials as biological lubricant additives for artificial joints in the future.