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A multifunctional carboxylate-rich magnetic chitosan flocculant (Mag@PIA-g-CS) was prepared through surface graft copolymerization on magnetite particles. The effect of monomer molar ratio, initiator and pre-neutralized degree on polymerization rate was determined. Various analytical methods were applied to characterize Mag@PIA-g-CS, exhibiting the successful grafting of polymers, good magnetic feature and core-shell structure. The kinetic process of Ni(II) and malachite green (MG) flocculation by Mag@PIA-g-CS reached equilibrium within <60 min with the optimal uptake rate of 98.3% and 87.4%, and exhibited satisfactory removal effect in wide pH range (4.0–8.0 for Ni(II), 5.0–10.0 for MG). Mag@PIA-g-CS exhibited superior flocculation performance over chitosan magnetic flocculant (Mag@CS). The pH-dependent behavior, rapid responsiveness and sensitivity to ionic strength in batch flocculation tests indicated the distinct effect of ionic groups. Moreover, sweeping action of linear molecular chains facilitated further flocculation. Mag@PIA-g-CS showed high stability in extreme environments, and can be easily regenerated and separated. [ABSTRACT FROM AUTHOR]