Carboxylated cross-linked chitosan beads (CCB) showed a significant defluoridation capacity (DC) of 1385 mgF(-)/kg than the raw chitosan beads (CB) which displayed only 52 mgF(-)/kg. Sorption experiments were performed by varying contact time, pH, presence of co-anions and temperature. The nature and morphology of the sorbent were discussed using FTIR and SEM with EDAX analysis. The stability of the beads in solution was explained in terms of swelling ratio of the beads. The fluoride uptake onto CCB obeys both Freundlich and Langmuir isotherms. Thermodynamic studies revealed that the nature of fluoride sorption is spontaneous and endothermic. Sorption kinetics is mainly controlled by pseudo-second-order and intraparticle diffusion models. 0.1M HCl was identified as the best eluent. The suitability of CCB at field conditions has been tested with field sample collected from a nearby fluoride-endemic area.