This study investigated the initiation and maintenance of nitritation in a membrane bioreactor (MBR) with long solids retention time (SRT) of 43.8 days. Nitritation was initiated within 65 days in the MBR via dissolved oxygen (DO) limitation (<0.5 mg/L). However, nitrite oxidizing bacteria (NOB) (Nitrospira and Nitrobacter) acclimated to the low DO environment and proliferated from day 81, leading to nitrate accumulation. Thereafter, the combined strategy of DO limitation and in-situ generated free nitrous acid (FNA) shock successfully restored and maintained stable nitritation for >70 days. Quantitative polymerase chain reaction (qPCR) results showed that cell abundances of Nitrospira and Nitrobacter decreased by between 50.0 to 68.9% and 60.6 to 96.4%, respectively following the FNA shocks. The maximum ammonium loading rate achieved was 1.81 kg N/(m3 day) with ammonium removal ratio and nitrite accumulation ratio of over 0.97 and 0.96, respectively. Average emission rate of N2O from the MBR was 2.1 ± 0.72% of ammonium removed. FNA shock on day 195 reduced the N2O emission by 13.6%. The strategy developed in this study verified that spiked FNA shock together with DO limitation can be used for maintaining nitritation in MBRs with long SRTs. This method can potentially allow for maintaining nitritation at relatively low capital and operating expenditure when treating high concentration ammonium wastewater.