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In view of the problems surrounding the research and application of carbon materials, the process of choosing a carbon source is still not perfect. There are few studies concentrating on the establishment of structure–property relationships based on the choice of carbon source. In this regard, our present work contributes the design of an organic precursor that is expected to allow the controllable construction of the carbon material, thus regulating its functionality. A highly π-conjugated Schiff base moiety with alternating imine groups (C＝N) and benzene rings was incorporated into the main chain of a mesoporous polymer. For comparison, a bisphenol-A-type moiety was employed in the main chain of another mesoporous polymer. Using the mesoporous polymers as organic precursors for porous carbon sources, the formation of mesoporous carbon can be attributed to the presence of the highly π-conjugated Schiff base moiety due to its self-supporting effect and char-forming ability, which are absent in the bisphenol-A-type moiety. However, we are not only concerned with the contribution from the chemical structure of the designed precursor to the controllable construction of mesoporous carbon, but also concerned with its regulation of the electrochemical performance of the resulting material. Through characterization using cyclic voltammetry (CV), galvanostatic charge–discharge profiles, and electrochemical impedance spectroscopy (EIS), this kind of mesoporous carbon has been found to have excellent charge storage and transportation abilities and shows potential for application in the electrodes of electrochemical capacitors. [ABSTRACT FROM AUTHOR]