The　pervasive　presence　of　antibiotics　in　the　environment　poses　ecological　risks　and　jeopardizes　human　health.　Herein,　a　simple　one-step　hydrothermal　method　was　used　to　prepare　a　boron-doped　(B-doped)　bimetallic　carbon　felt　as　a　cathode　for　the　heterogeneous　electro-Fenton　(HEF)　system.　In　the　HEF　process,　the　modified　electrode　(B-Co/Fe@CF)　demonstrated　exceptional　efficiency　in　degrading　the　target　pollutant　doxycycline　(DOX),　owing　to　its　maximal　degree　of　defect　and　minimal　electrochemical　impedance.　In　addition,　XPS　and　structure-activity　relationship　analysis　results　revealed　that　the　superior　performance　of　the　modified　electrode　stemmed　from　the　predominant　influence　of　sp(3)/sp(2),　C=O　and　metal-boron　(M-B)　groups　in　initiating　the　production　of　H2O2　and　the　consequent　formation　of　reactive　oxygen　species　(ROS).　Meanwhile,　the　introduction　of　non-metallic　boron　species　significantly　accelerated　the　sustainable　cycling　of　Co(II)/Co(III)　and　Fe(II)/Fe(III).　The　quenching　and　probe　experiments　suggested　that　the　radicals　center　dot　O-2(-)　and　center　dot　OH　significantly　contributed　to　the　elimination　of　DOX.　Moreover,　the　advanced　B-Co/Fe@CF-HEF　system　exhibited　remarkable　versatility,　stability　and　effectiveness　throughout　the　degradation　process.　Three　pathways　for　the　degradation　of　the　pollutants　were　identified　using　density　functional　theory　(DFT)　calculations　and　LC-MS　detection.　Additionally,　the　treated　DOX　solution　significantly　reduced　the　toxicity　to　the　growth　of　E.　coli　and　mung　bean　in　actual　toxicity　experiments.　This　research　presented　a　novel　outlook　on　developing　the　B-doped　metal　catalysts　for　efficient　degradation　of　pollutants　and　showcased　promising　applications　in　organic　wastewater　treatment.