Bioaugmentation was used to upgrade the nitrification process in a full-scale municipal WWTP with an A(2)/O system. A mixture of nitrifying bacteria was inoculated into the bioreactor for a final concentration of 1% (v/v). The upgrade process took 25 days, and the NH4+-N removals reached 94.6% (increased at least by 75%). The effluent concentrations of COD and NH4+-N stabilized at < 30 mg/L and < 4 mg/L even when the corresponding influent concentrations were over 300 mg/L and 60 mg/L, which met the first-class requirement of the National Municipal Wastewater Discharge Standards of China (COD <= 50 mg/L, NH4+-N <= 5 mg/L). The succession of the microbial community showed the enhanced NH4+-N removal efficiency mainly resulted from the persistence of introduced ammonia-oxidizing bacteria (AOB) and nitrite-oxidizing bacteria (NOB), which increased from 0% to 0.4% and from 0.01% to 2.1%, respectively. This bioaugmentation was shown as an effective technology for upgrading or retrofitting conventional systems to tertiary-level.