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• Formation mechanisms of PFRs in BC are reviewed. • Catalytic role of BC-PFRs in environmental pollution remediation is evaluated. • BC-PFRs systems include redox, advanced oxidation, photocatalytic, and sonocatalytic system. • Future challenges of BC-PFRs in environmental pollution remediation are proposed. Biochar as an emerging carbonaceous material has exhibited a great potential in environmental application for its perfect adsorption ability. However, there are abundant persistent free radicals (PFRs) in biochar, so the direct and indirect PFRs-mediated removal of organic and inorganic contaminants by biochar was widely reported. In order to comprehend deeply the formation of PFRs in biochar and their interactions with contaminants, this paper reviews the formation mechanisms of PFRs in biochar and the PFRs-mediated environmental applications of biochar in recent years. Finally, future challenges in this field are also proposed. This review provides a more comprehensive understanding on the emerging applications of biochar from the viewpoint of the catalytic role of PFRs. [Display omitted] [ABSTRACT FROM AUTHOR]