Aerobic granular sludge (AGS) is a special type of biofilm formed by the self-aggregation of microorganisms and extracellular polymers and is considered a promising technology for wastewater treatment. However, new strategies are still being proposed as to how to improve the extracellular polymeric substances (EPS) production that influences the formation of AGS. Recently, the acceleration of aerobic granulation using autoinducers such as N-acyl-homoserine lactone (AHL)-mediated quorum sensing has been reported. However, it is not yet fully understood due to knowledge gaps on the correlations depending on the type of AHL used. In this study, to evaluate the effects of various AHL on the AGS formation of activated sludge, the secretion of extracellular polymeric substances, biofilm formation, and sludge characteristics were comprehensively investigated. Among the AHL types, tightly bound EPS (TB-EPS) and loosely bound EPS (LB-EPS) in the reactor with C8-HSL added were 18.49 and 74.07 mg/g VSS, respectively, which represented increases of 3.15% and 53.76% compared to the control group. Additionally, C8-HSL increased the relative hydrophobicity and biomass volume by 153% and 218%, respectively. As a result, AHL had a positive effect on biomass content, an increase in sludge size, and an improvement in sludge sedimentation in the early stage of granulation, and C8-HSL was found to be the most suitable for initial granulation among AHL types.