The defluoridation capacity (DC) of a chelating resin, namely Indion FR 10 (IND), and Ceralite IRA 400 (CER), an anion-exchange resin, were compared under various equilibrating conditions for the identification of selective sorbent. The results showed that chelating resin is more selective than an anion-exchange resin for fluoride removal. The fluoride sorption was reasonably explained using Freundlich and Langmuir isotherms. The surface morphology of resins before and after fluoride sorption was observed using scanning electron microscopy (SEM). Fourier transform infrared spectroscopy (FTIR) was used for the determination of functional groups responsible for fluoride sorption. Various thermodynamic parameters such as DeltaG0, DeltaH0, DeltaS0, and Ea have been calculated to understand the nature of sorption. The sorption kinetic mechanism was studied with reaction-based and diffusion-based models. The sorption process was found to be controlled by pseudo-second-order and particle diffusion models. The performance of the resins studied has been tested with field samples collected from a fluoride-endemic area.