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Waste activated sludge (WAS), which is rich in organic substances, provides an energy resource. To recover hydrogen from the organic wastes, microbial electrolysis cell may be used as an efficient device. Since different extra applied voltages have significant effects on the efficiency of microbial electrolysis cell, this paper explores different extra applied voltages (0.6 V–1.2 V) affecting the utilization of sludge fermentation liquid (SFL) that is treated with synchronous double-frequency (28 + 40 kHz) and alkali coupling 72-bacth mesothermal anaerobic fermentation (35 °C). It is found that 0.8 V was the optimum extra applied voltage. With this voltage, the highest energy recovery efficiency will be 169 ± 1% and the peak of soluble chemical oxygen demand (SCOD) removal efficiency can be found at 51.4 ± 0.6%; Coulombic efficiency is 98.9 ± 1.0%. The order of complex matter consumption is found to be HAc > HPr > n HBu > n HVa > total carbohydrates > protein. The processing methods of synchronous double-frequency, alkaline, coupling with anaerobic fermentation are feasible for microbial electrolysis cell to transform large amount of waste activated sludge into energy.