Electrochemical　advanced　oxidation　processes　(EAOPs)　are　favorable　technologies　to　remove　organic　wastewater,　but　the　development　of　high-efficiency　and　low-energy　consumption　anode　catalysts　is　still　a　priority.　Herein,　a　carbon　cloth-supported　MnS/MnO2　heterostructure　rich　in　oxygen　vacancies　is　successfully　synthesized　as　an　anode　for　the　electrocatalytic　removal　of　methyl　orange　(MO)　wastewater.　The　anode　catalyst　possesses　lower　charge　transfer　resistance　(77.4　Ω),　higher　oxygen　evolution　potential　(2.13　V　vs　RHE),　and　removes　nearly　100%　methyl　orange　(20　mg/L)　in　30　min　with　a　high　mineralization　current　efficiency　of　73.2%　and　low　energy　consumption　of　23.4　kWh/kg　TOC.　Through　density　functional　theory　(DFT)　studies,　oxygen　vacancies　increase　the　positive　charge　of　Mn　atoms　in　the　vicinity　of　the　heterostructure　interface,　thus　improving　its　catalyst　activity.　The　calculated　adsorption　energy　of　H2O　(ΔEH2O)　is　reduced　from　−　0.672　eV　for　MnO2　to　−　0.887　eV　for　oxygen-vacancy　heterostructure,　which　is　conducive　to　the　water　splitting　to　form　•OH.　Overall,　this　study　provides　a　promising　strategy　for　enhancing　the　electrocatalytic　removal　performance　of　manganese　dioxide　by　using　heterostructure　design　and　oxygen　vacancy　engineering.　©　2023　Elsevier　B.V.