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Magnetic separation technology is an efficient and feasible way to achieve rapid recovery of adsorbents, thus, the use of magnetic adsorbents has attracted the attention of many researchers. However, currently reported magnetic adsorbents have limited adsorption capacity due to insufficient adsorption sites and reactive groups. In this work, a novel magnetic chitosan-based amphiphilic adsorbent (PFSC) was synthesized by using UV-light irradiation method to combine with acryloyloxyethyl dimethylbenzyl ammonium chloride (AO), a molecule containing benzyl groups. PFSC and its precursors were carefully characterized, and their adsorption performances for the removal of anionic dyes were explored. The characterization results showed that the magnetic copolymers with a type of microsphere structure were successfully synthesized. Moreover, PFSC exhibited superior adsorption efficiency and pH resistance compared to those of an unmodified chitosan-based magnetic adsorbent (FSC). The maximum adsorption capacities of PFSC towards orange II (OG), acid red 88 (AE) and red amaranth (RM) were 955.0, 1075.8 and 567.5 mg/g at pH 3.0, respectively. The adsorption kinetics and isotherms of PFSC were consistent with that of a pseudo-second order kinetic model and the Langmuir isotherm model. In addition, adsorption-desorption experiments showed that PFSC could be rapidly separated and efficiently recycled even after 4 uses. More importantly, the FTIR and XPS results revealed that electrostatic adsorption and π-π stacking interactions were the main adsorption mechanisms for the PFSC-enhanced removal of anionic dyes. [Display omitted] • The chitosan-based amphiphilic magnetic copolymer was successfully synthesized by the UV-light initiated method. • The novel magnetic copolymer can be easily separated from solution by magnetic force. • The enhanced electrostatic adsorption and π-π stacking effect played an important role in the removal of anionic dyes. • The novel magnetic copolymer can be reused by simple acid-alkali adjustment. [ABSTRACT FROM AUTHOR]