A new derivative of chitosan functionalized with chloroacyl chloride and 2-(2-aminoethylamino) ethanol was synthesized for the preparation of a magnetic nanocomposite containing Fe3O4@TiO2 nanoparticles. Characterizations were done by Fourier transform infrared spectroscopy (FT-IR), X-ray diffraction (XRD), scanning electron microscopy (SEM), thermogravimetric analysis (TGA), and vibrating sample magnetometer (VSM). The nanocomposite was examined for the defluoridation of water, and the effect of contact time, pH, initial fluoride ion concentration, and adsorbent dosage were investigated. The Langmuir model showed the best agreement with the experimental data. The maximum adsorption capacity for the fluoride removal from aqueous solutions was 15.385 mg/g at 318 K and pH = 5.0. The adsorption mechanism matches the pseudo-second-order kinetic model with a rate constant (k2) of 0.68 g/mg·min. The thermodynamics study of the nature of adsorption showed that ΔH and ΔS were 13.767 kJ/mol and 0.066 kJ/mol·K respectively. A mechanism for the fluoride sorption was proposed by considering the electrostatic and hydrogen bonding interactions.