The　incorporation　of　redox-active　anions　into　aqueous　electrolytes　endows　electrodes　with　enhanced　specific　energy　density　for　supercapacitors.　However,　the　congruent　relationship　between　the　redox　chemistry　of　electrolytes　and　electrode　surfaces　is　still　not　well　understood.　Herein,　two-dimensional　nitrogen-doped　porous　carbon　nanosheets　(denoted　as　NC-x　with　x　being　the　carbonization　temperature　in　Degree　Celsius)　are　systematically　synthesized　by　using　general　dual-crystals　templating　assisted　strategy　with　pore　structure　and　surface　composition　optimized.　Employed　as　both　positive　and　negative　electrodes,　the　as-prepared　NC-900　with　a　large　specific　surface　area　and　ample　graphitic　N　sites　shows　a　high　specific　capacitance　of　251　F　g−1　with　a　voltage　window　of　1.6　V　and　energy　density　of　22.4　Wh　kg−1　associated　with　86.5%　capacity　retention　after　30,000　cycles　using　aqueous　iodide　redox　electrolyte.　The　experimental　and　theoretical　analyses　reveal　the　contributions　of　nitrogen　configurations　on　the　carbon　scaffolds　to　accelerate　the　redox　chemistry　of　iodides.　The　enhanced　redox　performance　of　the　porous　carbon　nanosheets　is　linearly　proportional　to　the　graphitic　N　content,　which　is　consistent　with　the　large　electron-donating　area　and　the　strong　adsorption　capacity　towards　iodine　species　at　the　graphitic　N　sites.　This　work　shows　a　new　design　strategy　of　carbon　electrodes　for　high-performance　supercapacitors　with　the　aqueous　redox　electrolytes.　©　2022　Elsevier　B.V.