Aerobic granular sludge is a form of microbial auto-aggregation, and a promising biotechnology for wastewater treatment. This review aims at providing the first comprehensive, systematic, and in-depth overview on the application of aerobic granules as biosorbents. The target pollutants encompass heavy metals (both cationic and oxyanionic), nuclides, dyes, and inorganic non-metal substances. Different granule types are discussed, i.e. intact and fragmented, compact and fluffy, original and modified, and the effects of granule surface modification are introduced. A detailed comparison is conducted on the characteristics of granular biomass, the conditions of the adsorption tests, and the resultant performance towards various sorbates. Analytical and mathematical tools typically employed are presented, and possible interactions between the pollutants and granules are theorized, leading to an analysis on the mechanisms of the adsorption processes. Original granules appear highly effective towards cationic metals, while surface modification by organic and inorganic agents can expand their applicability to other pollutants. Combined with their advantages of high mechanical strength, density, and settling speed, aerobic granules possess exceptional potential in real wastewater treatment as biosorbents. Possible future research, both fundamental and practical, is suggested to gain more insights into the mechanism of their function, and to advance their industrial application.