Aerobic granular sludge (AGS) can achieve simultaneous carbon, nitrogen and phosphorus removal owing to its three-dimensional oxygen gradient structure. However, long start-up period and poor operational stability restrict its application and promotion. A novel rapid granulation strategy, viz., the short-term (7 days) addition of ferric chloride at the commissioning stage, was developed and verified in this study. The granulation period was shortened by 9 days, and the formed granules were compact and dense with an Fe concentration of 250 mg L. The addition of flocculant not only maintained a high sludge concentration during the initial stages of granulation (5.3 g L), but also stimulated the secretion of TB-EPS and increased protein and polysaccharide contents, thereby expediting granule formation. Additionally, ferric chloride induced a diverse microbial community in granules, resulting in the emergence of new genera, such as Thaurea, Brevundimonas and Kinneretia, which improved pollutant removal performance and flocculent aggregation. The removal efficiencies of COD, PO-P, and NH-N stabilized at 94.2, 62.4, and 71.3%, respectively. Therefore, it has been demonstrated that short-term ferric chloride dosing has a synergistic effect on aerobic granulation.