Mineralization of aqueous alkylbenzenesulfonates (ABS) was investigated by means of contact glow discharge electrolysis (CGDE). Toluenesulfonic and dodecylbenzenesulfonic acids in a neutral phosphate buffer solution were smoothly degraded and eventually converted to inorganic carbon and sulfate ion when CGDE was conducted under the applied DC voltage of 500 V and current of ca. 90 mA. As the intermediate products, some phenolic compounds were detected as well as carboxylic acids such as oxalate, formate and so on. It was demonstrated that the decay of ABS followed the first-order rate law. Based on the detailed analysis of the hydroxylation products and kinetic consideration, it was assumed that hydroxyl radicals would play a crucial role in the oxidative degradation of aqueous ABS. The features of CGDE as a tool for the removal of organic pollutants in water were discussed in comparison with other physicochemical methods.