There is an overwhelming desire to develop new sulfide oxidation electrocatalysts that perform at low potentials and exhibit high current density for the removal and efficient sensing of sulfide. This article describes a comparative electrochemical analysis of various commercially available carbon materials and polymer/surfactant composite electrocatalysts for direct electrooxidation of sulfide in an aqueous solution. The composites were prepared from five different carbon materials multiwalled carbon nanotubes, fullerene‐C60, graphene, glassy carbon, and carbon nanofibers (CNF) and four different polymers: chitosan, polyvinylidene fluoride, Nafion, and indigenously synthesized poly[2‐(methacryloyloxy)ethyl] trimethylammonium chloride (PMTC). The carbon@polymer composites were prepared by a simple ultrasonication technique, and the electrodes were prepared by drop‐drying the prepared composite on indium tin oxide (ITO) substrates. The CNF@PMTC showed the highest positive zeta potential that allowed an accumulation of many negatively charged sulfide ions at the CNF@PMTC surface. Cyclic voltammetry was used for the electrooxidation of sulfide in an aqueous solution of tris buffer (0.05 M; pH 8.0) and KNO3 (0.1 M). The lowest sulfide oxidation peak potential (i. e., −51 mV vs. standard hydrogen electrode) with a high catalytic current response (730 μA/cm2) of the CNF@PMTC‐modified ITO electrode among the tested and previously reported carbon‐based electrode materials make it ideal for direct sulfide electrooxidation. Taking this and its simple preparation method into account, CNF@PMTC can be considered a benchmark carbon‐based electrocatalyst for sulfide oxidation.