Since high degradation efficiency and environmental friendliness, the Electro-Fenton technology has been widely applied to remove antibiotics in wastewater. In-situ loading of electrochemically active metals on graphite felt (GF) is considered as a promising strategy for improving its electrocatalytic activity and reusability. Here, a series of Mn/Co MOFs derivatives modified graphite felt cathodes (MnxCo3-x@C-GF) were fabricated without any binder, which was used for the treatment of ciprofloxacin (CIP). The morphology, pore structure and electrochemical activity of MnxCo3-x@C-GF changed by adjusting the ratio of Mn/Co in the MOF-74 precursor. Owning to the optimized Mn/Co ratio, Mn2Co1@C-GF exhibited the most excellent catalytic ability with hierarchical porous structure and faster electron transfer. The results showed that the CIP degradation efficiency could reach 99.8% in 60 min. Mn2+/3+/4+ and Co3+/2+ enhanced the generation of active radicals (·OH) by Fenton-like reaction and further improved degradation performance. In addition, the cathode had maintained good stability during four cycles. This work provides an alternative strategy for fabricating efficient self-supporting cathode materials in the future.