In this study, the effect on the stability of Aerobic Granular Sludge (AGS) with different Carbon/Nitrogen (C/N) ratios was investigated. The C/N ratios were controlled to 10.0, 7.5, 5.0, and 2.5 using the sequencing batch reactor, and the results showed that the removal efficiency of organic matter and total nitrogen decreased simultaneously with the decrease of C/N ratio. The removal efficiency of organic matter and total nitrogen at C/N ratio of 2.5 was 70.7% and 52.3% respectively. In addition, the AGS/mixed liquor suspended solids (MLSS) ratio showed a tendency to decrease from 85.7% to 73.7%, while the sludge volume index showed a tendency to increase from 82 mL/g to 102 mL/g as the C/N ratio decreased. At the same time, the apparent deviation of polysaccharide (PS) content in extracellular polymeric substances was observed, and polysaccharides/protein (PS/PN) ratio decreased from 0.62 to 0.31 as the C/N ratio decreased. Optical microscope observations showed that the reduction in C/N ratio caused the growth of filamentous bacteria and significantly affected the stability of AGS.