Carbon-based metallic catalysts (CMCs) have emerged as efficient materials for removing water contaminants,but preparing CMCs with high efficiency and stability remains a great challenge. In this study, weprepared a bimetallic composite of Cu-Co/C catalyst via a gelation and calcination method to degradeOrange II by activating peroxymonosulfate (PMS). The characterization results demonstrated that thespecific surface area and pore size of Cu-Co/C catalysts were 1.675 m2/g and 6.313 nm, respectively,which can provide larger catalytic active sites for boosting PMS activation. Moreover, the effects of differentfactors on Orange II degradation efficiency, cyclic experiments, and possible application in realwater bodies were investigated. The Cu-Co/C catalyst can effectively activate PMS, and 50 mg/L ofOrange II was almost completely removed within 15 min. Additionally, the Cu-Co/C catalyst exhibitedhigh degradation efficiency for other organic dye pollutants. The radical quenching experiments indicatedthat the main active species for Cu-Co/C catalyzed degradation of Orange II were SO4and singlet oxygen(1O2). The catalyst demonstrated good stability and performance in real water bodies. We believe thatthis study will promote the application of carbon-based bimetallic catalysts in the environmental remediationprocess that utilize SO4based advanced oxidation.