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In this study, top-down synthesis of sulfur-doped graphene nanosheets (SDGNs) by simple electrochemical exfoliation was explored as a means of producing metal-free electrocatalysts for oxygen reduction and oxygen evolution reactions (ORR and OER, respectively). In a typical procedure, graphite foils were used to obtain bulk quantities of SDGN catalysts in the presence of thiosulfate as a sulfur source. Highly stable colloidal dispersions of SDGNs were obtained by applying a voltage of 15 V at an optimized Na 2 S 2 O 3 :H 2 SO 4 molar ratio of 5 : 1 (denoted SDGN(5)). Physicochemical characterizations by Raman spectroscopy, transmission electron microscopy, X-ray diffraction, and X-ray photoelectron spectroscopy confirmed the existence of sulfur and its electronic/structural properties in graphene nanosheets. In alkaline media, SDGN(5)-modified electrodes were comparable or superior to pristine graphene and a benchmark commercial platinum-based electrodes in terms of stability, methanol tolerance, n values, and onset potential for ORR and OER. The specific capacitance (149.9 F g−1) of SDGN(5) supported its excellent ORR/OER performance and enhanced surface area. [ABSTRACT FROM AUTHOR]