Engineering　multicomponent　electroactive　materials　is　an　effective　strategy　to　improve　electrochemical　performance　by　adjusting　the　atomic　and　electronic　structure.　In　this　work,　we　directly　synthesize　oriented　bimetallic　CoNi-MOF　nanosheets　on　CFP　(carbon　fiber　paper).　The　CoNi-MOF/CFP　shows　high　specific　capacitance,　outstanding　rate　capability　and　long-term　cycling　stability　compared　to　a　monometallic　Ni-MOF　or　Co-MOF.　By　adjusting　the　Co/Ni　molar　ratio,　CoNi23/CFP　(Co　:　Ni　=　2　:　3)　displays　the　highest　specific　capacitance　(2033　F　g(-1)　at　1　A　g(-1)).　The　introduction　of　Co　into　the　Ni-MOF　matrix　shortens　Co/Ni-centered　bond　distances,　resulting　in　improved　bond　strength,　facilitating　the　charge　transfer　and　increasing　the　electrical　conductivity　of　the　CoNi-MOF,　which　were　proved　by　X-ray　absorption　fine　structure　(XAFS)　spectroscopy,　high　angle　annular　dark　field　(HAADF)　imaging,　and　electrochemical　impedance　spectroscopy　(EIS).　Our　study　demonstrates　the　origin　of　performance　improvements　and,　therefore,　may　provide　a　feasible　scheme　to　unlock　high-performance　MOF　electrode　materials.