In order to accelerate the aerobic granulation and thus promote the degradation efficiency of highly refractory compounds such as pyridine in aerobic granular system, enhanced aerobic granulation based on biochar addition was developed in this study. The results indicated that the sludge formed in the reactor with the addition of biochar possessed excellent settling property, high biomass retention and excellent degradation ability. Extracellular polymeric substances (EPS) contents in granular sludge increased noticeably at the presence of biochar, indicating the stimulation of EPS secretion by biochar. High throughput sequencing analysis exhibited that enhanced granulation and pyridine degradation could be attributed to the enrichment of aggregation-related species and pyridine degrading species at the presence of biochar. This study indicated that adding biochar is a simple and effective method for the initiation of granulation to facilitate the treatment of high-strength refractory wastewater.