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• Multifunctional magnetic composite nanoparticles were facilely prepared. • The as-prepared FS@CS-PAA showed excellent adsorption capacities for cationic dyes. • FS@CS-PAA exhibited satisfactory removal rates for metal ions in a wide pH range. • The good adsorption ability was attributed to abundant active sites from CS-PAA. • FS@CS-PAA's good stability and reusability facilitated its practical application. Wastewater containing highly toxic, non-biodegradable and carcinogenic organic dyes and metal ions has been regarded as a severe threat to ecological environment and human health. Thus, it is of great significance to develop an effective approach to purify this kind of wastewater. Herein, novel magnetic adsorbent FS@CS-PAA was facilely prepared by coating anionic polyacrylamide-modified chitosan (CS-PAA) on the surface of silica-combined Fe 3 O 4 (FS). The morphology, structure, physic-chemical and magnetic properties of as-prepared FS@CS-PAA were fully characterized by various characterization techniques. Its adsorption behaviors towards cationic dyes and metal ions were systematically investigated in single systems, binary systems, and model wastewater. FS@CS-PAA was proved to have superior adsorption capacities of 2330.17 and 1044.06 mg g−1 respectively for crystal violet and methylene blue at 318.15 K, much higher than other reported adsorbents. Besides, FS@CS-PAA exhibited a pH-independent adsorption capability for metal ions, as demonstrated in single systems and in metal ion-dye binary systems, thus it could be used to treat a variety of metal ion wastewaters with different pH values. Moreover, FS@CS-PAA could be effectively and easily regenerated by HCl solution after the treatments of both synthetic wastewater and model wastewater. As revealed in FTIR and XPS analyses, the adsorption mechanism was mainly attributed to the electrostatic interaction, hydrogen bonding, cation exchange and chelating effect. With its excellent adsorption capacity for cationic dyes, pH-independent adsorption capability for metal ions, easy separation ability, satisfactory stability and good reusability, FS@CS-PAA can become an ideal candidate for wastewater treatment. [ABSTRACT FROM AUTHOR]