Great　disparity　in　crystal　size　and　incompatibility　in　crystal　interface　of　catalysts　lead　to　low　catalytic　activity,　restricting　its　application　for　antibiotic　degradation.　Herein,　a　dual　regulation　strategy　via　intrinsic　ion　interpenetration　was　proposed　to　engineer　multifunctional　nano-interfacial　BiFeVO4/NH2-MIL-88B(Fe-Bi)　(BFV/NMFB)　catalysts　for　efficient　photo-Fenton-like　catalytic　degradation　OTC.　These　multifunctional　nano-interfaces　(Fe-O-Bi)　with　abundant　vacancy　defects　enhanced　electrical　conductivity,　broadened　light　absorption　and　narrowed　band　gap.　Furthermore,　the　strong　interface　bonds　enhanced　H2O2　adsorption　and　activation,　accelerated　photogenerated　carrier　separation/transfer　and　promoted　Fe3+/Fe2+　redox　activity.　These　properties　gave　an　excellent　synergistic　effect　of　photo　and　Fenton-like　catalysis　(synergy　factor　up　to　4.6)　via　changing　photocurrent　transfer　pathway　and　interfacial　adsorption-activation　mechanism.　Therefore,　the　designed　BFV/NMFB　exhibited　superior　photo-Fenton-like　catalytic　activity　(k(a)　=　189　mol.mg(-1).min(-1)),　about　3.6-58　times　higher　than　these　of　reported　catalysts.　The　proposed　strategy　provided　a　promising　method　for　the　design　of　MOFs　composition　for　application　of　antibiotic　degradation.