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Nitrogen-doped mesoporous carbon/poly-o-phenylenediamine composites (denoted as N-MC/PoPD) were successfully synthesized by sacrificial hard template method followed by in situ oxidation polymerization initiated by FeCl _3 . It is revealed that the resultant N-MC/PoPD composites still remained original graphitization structure and narrow pore size distributions (centered at ∼3.8 nm) but suffered visibly monotonical decrease in specific surface area after oPD was increasingly polymerized onto N-MC with an increase of the mass ratio of PoPD to N-MC from 1:1 to 5:1. As supercapacitor electrode measured by galvanostatic charge-discharge in 6 mol L ^−1 KOH, a volcano curve was found when plotting specific capacitance of the N-MC/PoPD versus the mass ratio of N-MC to oPD; the N-MC/PoPD(2:1) with moderate surface area and the highest electrochemical conductivity delivered the highest specific capacitance of 229 F g ^−1 at a current density of 1 A g ^−1 , which is twice of that obtained on the single N-MC with the maximum surface area. The remarkable enhancement in specific capacitance could be ascribed to the synergistic effect between two components of N-MC and PoPD.