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In this work, a novel chitosan-based magnetic adsorbent [poly(2-(dimethylamino)ethyl methacrylate) grafted magnetic chitosan microspheres, GMCMs] was synthesized by graft polymerization of (2-(dimethylamino)ethyl methacrylate on the surface of magnetic chitosan microspheres (MCMs). The as-prepared GMCMs exhibited significantly enhanced adsorption capacity towards anionic dyes (e.g., Acid Green 25 and Reactive Blue 19) compared with MCMs. It is due to the fact that the abundant tertiary amine groups of the grafted polymer protonated at low pH and the polymer chains stretched as a result of electrostatic repulsions and chain-solvent interactions. The stretched polymer chains provided a variety of adsorption sites, which efficiently adsorbed dyes through electrostatic interactions and hydrogen bonding. While, in alkaline conditions, the tertiary amine groups were deprotonated and the polymer chains collapsed due to hydrophobic interactions, which facilitated the regeneration of the dye-loaded GMCMs at high pH. The regenerated GMCMs showed excellent adsorption performance even after five adsorption–desorption cycles. Besides, the GMCMs could be rapidly separated from aqueous solutions under an external magnetic field. Therefore, the GMCMs materials bear great application potentials in water treatment owing to its high adsorption capacity, pH-responsiveness, facile regeneration and good reusability. [ABSTRACT FROM AUTHOR]