The carboxylated chitosan beads (CCB), which have a defluoridation capacity (DC) of 1385 mg F(-)/kg, have been further chemically modified by incorporating La(3+) ion (La-CCB) and its DC was found to be 4711 mg F(-)/kg whereas the raw chitosan beads (CB) possess only 52 mg F(-)/kg. The fluoride removal by La-CCB is governed by both adsorption and complexation mechanism. The functional groups present in beads were identified by FTIR analysis. The surface condition and existence of fluoride on the beads was confirmed by SEM with EDAX analysis. The experimental data have been analyzed using Freundlich and Langmuir isotherm models. Thermodynamic parameters such as DeltaG(o), DeltaH(o) and DeltaS(o) were calculated to predict the nature of sorption. The kinetic studies were investigated with reaction-based and diffusion-based models. A field trial was carried out with fluoride water collected from a nearby fluoride-endemic village.