The titration of the interfacial capacitance of a C-cloth electrochemical capacitor electrode was undertaken for the purpose of evaluating the cyclic voltammetry (CV) responses as a function of the pH of an aqueous electrolyte over the range of 0–14. As the pH was increased from 0 (aqueous H2SO4) to a progressively more alkaline (NaOH) solution of pH 11, a 30% loss in capacitance is seen, partly attributable to the disappearance of the pseudocapacitive peaks based on the oxidation/reduction of the surface quinone groups. As the pH is increased above 11, the capacitance increases ca. 20%, as other surface functionalities (a pyrone derivative and another unknown species) become activated in alkaline solution. When the C-cloth is titrated from pHs of 14 to 2, the CV current profile shrinks (with a concomitant decrease in charge-storage capacity). However, at electrolyte pHs below ca. 2, the quinone functionalities are activated and the charge-storage capacity increases ca. 30% above the initial value. It was found that the CV current responses in pH 14 electrolytes are smaller when the titration is base-initiated, rather than acid-initiated, due to an activation step required to make the pyrone functionalities active in alkaline solution.