Eutrophication has increased globally which has resulted in a deterioration of water quality, largely due to an increase nitrogen and phosphorus from urban sewage. In this study, a novel A2/O process to simultaneously remove nitrogen and phosphorus from wastewater is presented which could overcome issues regarding insufficient carbon sources, and maximizing the use carbon sources. Moreover, the carbon source could not meet the required A2/O system, which aggravated the competition of carbon sources in the A2/O system. Methanol, glucose and ethanol were used as carbon sources with different ratios (3:0:0, 1:1:1, 0:2:1, 0:1:2, and 0:0:3) in the three chambers in the A2/O experiment. Results show that ethanol was the most efficient carbon source for removing nitrogen and phosphorus. Total nitrogen (TN) and total phosphorus (TP) removal rates were 78.23 and 78.18%, and the removal time of
NO2––N was 25 min. A dosing ratio of 0:1:2 (external carbon source) and a nitrate recycling ratio of 250% were then optimum conditions for the A2/O system, the A2/O system efficiently removed TN and TP. The removal rates of TN, NH3–N, and TP were 82.36, 96.67, and 92.18%, respectively. The effluent concentrations were 11.43, 4.1, and 0.45 mg/L, respectively, which reached the requirements of the type A standard GB18918‐2002. © 2018 American Institute of Chemical Engineers Environ Prog, 37: 1901–1907, 2018