In this research, a novel chitosan (CS)–vanadium-titanium-magnetite (VTM) composite was designed and synthesized. The interaction between CS-VTM and Congo red (CR) dye conformed to a pseudo-second-order model to support the potent involvement of chemisorption. The effects of adsorbent dosage, reaction temperature, and initial solution pH on adsorption of CR were investigated. Approximately 99.1% of CR (100 mg/L) was adsorbed at a CS-VTM dose of 2.0 g/L or above, while such a reaction was favored at temperatures of 65 °C and pH of 6.0. Thermodynamically, the adsorption of CR proceeded spontaneously (ΔG < 0) above 35 °C. According to scanning electron microscopy, X-ray photoelectron spectroscopy, Fourier transform infrared spectrometer, and zeta potential analysis, its adsorption on CS-VTM can be attributed to electrostatic attraction and hydrogen bonds. The prepared CS-VTM exhibited superior adsorption performance on removal of CR as evidenced by significantly large partition coefficient of 108.3 mg g−1 μM−1 (equilibrium adsorption capacity of 62.2 mg/g at CR dose of 100 mg/L). Overall, the CS-VTM proved to be a promising and environmentally friendly adsorbent for the highly efficient and effective removal of organic dyes among the comparable sorbents studied to date.
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