The　development　of　efficient　and　low-cost　bifunctional　electrocatalysts　for　oxygen　evolution　reaction　(OER)　and　hydrogen　evolution　reaction　(HER)　is　highly　desirable　for　electrochemical　energy　conversion.　Herein,　this　study　puts　forward　a　new　Co　decorated　N,B-codoped　interconnected　graphitic　carbon　and　carbon　nanotube　materials　(Co/NBC)　synthesized　by　direct　carbonization　of　a　cobalt-based　boron　imidazolate　framework.　It　is　demonstrated　that　the　carbonization　temperature　can　tune　the　surface　structure　and　component　of　the　resultant　materials　and　optimize　the　electrochemically　active　surface　area　to　expose　more　accessible　active　sites,　effectively　boosting　the　electrocatalytic　activity.　As　a　result,　the　optimized　Co/NBC　shows　superior　bifunctional　catalytic　activity　and　stability　toward　OER　and　HER　in　1.0　m　KOH　solution.　Furthermore,　the　catalyst　can　serve　as　both　the　anode　and　cathode　for　water　splitting　to　achieve　a　current　density　of　10　mA　cm−2　at　a　cell　voltage　of　1.68　V.　Experimental　results　and　theoretical　calculations　indicate　that　the　excellent　activity　of　Co/NBC　catalyst　benefits　from　the　synergistic　effect　of　partial　oxidation　of　metallic　cobalt,　conductive　N,B-codoped　graphitic　carbon　and　carbon　nanotube,　and　the　coupled　interactions　among　these　components.　This　work　opens　a　promising　avenue　toward　the　exploration　of　boron　imidazolate　frameworks　as　efficient　heteroatom-doped　catalysts　for　electrocatalysis.　©　2018　WILEY-VCH　Verlag　GmbH　&　Co.　KGaA,　Weinheim