Based on the improved high-efficiency sewage treatment performance of submerged membrane bioreactors (SMBRs), we focused on how to adjust the C/N ratio of the influent water during reactor start-up to prevent an excessive C/N ratio from causing membrane fouling. In this study, an experimental method of gradually adjusting the influent C/N ratio to quickly start the reactor was proposed, and the results showed that biofilm formation in R1 (SMBR, three influent C/N ratios of 5, 10, and 20) was approximately completed in 32 days, shorter than that (40 days) required in R2 (SMBR, influent C/N ratio of 20). Higher removal efficiencies of 76.4% for TN, 70.1% for COD, and 79.2% for NH3-N were obtained in R1 than in R2. The high-throughput sequencing results indicated that after 150 days of operation, the Shannon index of bacteria in R1 increased from 2.97 to 4.41 and the growth of Nakamurella, Ferruginibacter, and Rhodanobacter was promoted in the reactor, which indicated substantial microbial diversity in the biofilm. Therefore, gradually adjusting the influent C/N ratio could effectively enhance the nitrogen removal performance of denitrification microbial communities in SMBRs. This study offers a reliable approach for starting the SMBR-enhanced biological nutrient removal process in wastewater treatment plants by gradually adjusting the influent C/N ratio.