The development of excellent dye adsorbent with high adsorption capacity and good separation function is imperative to clean the wastewater. Herein, an innovative magnetic Fe-Fe 2 O 3 @poly(cyclotriphosphazene-co-polyethyleneimine) (named as Fe-Fe 2 O 3 @PCP) composite was fabricated through a facile copolymerization between hexachlorocyclotriphosphazene and polyethyleneimine in the presence of Fe-Fe 2 O 3 nanoparticles. With the help of scanning electron microscope, transmission electron microscope, Fourier transform infrared spectroscope and vibrating sample magnetometer, the microstructure of the resulting magnetic Fe-Fe 2 O 3 @PCP composite was characterized. Then, the adsorption performance of magnetic Fe-Fe 2 O 3 @PCP composite was evaluated by removing anionic dye acid chrome blue K (ACBK) from aqueous solution. The effects of contact time, initial solution pH and temperature on the adsorption of ACBK onto magnetic Fe-Fe 2 O 3 @PCP composite were systematically studied. The kinetics, isotherms and mechanism of the adsorption process were analyzed. Results show that the maximum adsorption capacity of the magnetic Fe-Fe 2 O 3 @PCP toward ACBK dye could be up to 260 mg g −1 at 25 °C in neutral solution. The adsorption kinetics follows both the pseudo-secondorder kinetic model and the Weber's intraparticle diffusion model well. And the Freundlich isotherm model can nicely fit the adsorption equilibrium data. The electrostatic attraction between Fe-Fe 2 O 3 @PCP and ACBK plays a dominant role in the adsorption process. Moreover, the magnetic Fe-Fe 2 O 3 @PCP composite owns a high saturation magnetization of 30.1 emu g −1 , rendering it rapid magnetic separability and good reusability. After five adsorption-desorption cycles, the magnetic composite still kept 75% of removal efficiency with the adsorption capacity of 195 mg g −1 . The excellent adsorption capacity and good magnetic separability make the magnetic Fe-Fe 2 O 3 @PCP composite a promising adsorbent for efficient removal of anionic dyes including ACBK from contaminated wastewater.