Chitosan beads (CB) as such have very low defluoridation capacity (DC) of 52mgF⁻/kg have been suitably modified by carboxylation followed by chelation with Fe³⁺ ion (Fe-CCB), in order to effectively utilize both hydroxyl and amine groups for defluoridation. The modified beads showed enhanced DC to a very significant level of 4230mgF⁻/kg. The fluoride removal process is governed by both adsorption and complexation mechanism. The sorbent was characterized using Fourier transform infrared spectrometer (FTIR) and scanning electron microscope (SEM) analysis. The experimental data have been analysed using isotherm and kinetic models. Thermodynamic parameters such as ΔG°, ΔH° and ΔS° were calculated to predict the nature of sorption. A field trial was carried out with fluoride water collected from a nearby fluoride-endemic village.