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Wastewater containing dyes poses a severe threat to human health and to environmental safety. Hence, finding an effective way to treat this wastewater has attracted wide attentions. In this study, quaternary ammonium group-rich magnetic nanoparticles (MNPs), Fe 3 O 4 @SiO 2 -MPS-g-DAC (FSMD), were facilely prepared by grafting polymerization and served as a cationic adsorbent to remove anionic dye Orange G from aqueous solutions. Being compared with Fe 3 O 4 @SiO 2 -MPS MNPs, the adsorption capacity of FSMD MNPs was notably enhanced and it could be maintained in a high level under a wide solution pH range. The dependency on pH and the sensitivity to ionic strength indicated that the main adsorption mechanism was the electrostatic interaction. The adsorption kinetics followed the pseudo-second-order model, and the adsorption isotherms were well described with the Langmuir model. According to the thermodynamic analysis, the adsorption process was spontaneous and endothermic. FSMD MNPs were proved to have advantages of fast adsorption rate, high adsorption capacity, easy separation ability under external magnetic field, and satisfactory reusability, therefore they can be applied in the removal of anionic dyes from wastewater. [ABSTRACT FROM AUTHOR]