Alumina possesses an appreciable defluoridation capacity (DC) of 1566 mg F-/kg. In order to improve its DC, it is aimed to prepare alumina polymeric composites using the chitosan. Alumina/chitosan (AlCs) composite was prepared by incorporating alumina particles in the chitosan polymeric matrix, which can be made into any desired form viz., beads, candles and membranes. AlCs composite displayed a maximum DC of 3809 mg F-/kg than the alumina and chitosan (52 mg F-/kg). The fluoride removal studies were carried out in batch mode to optimize the equilibrium parameters viz., contact time, pH, co-anions and temperature. The equilibrium data was fitted with Freundlich and Langmuir isotherms to find the best fit for the sorption process. The calculated values of thermodynamic parameters indicate the nature of sorption. The surface characterisation of the sorbent was performed by FTIR, AFM and SEM with EDAX analysis. A possible mechanism of fluoride sorption by AlCs composite has been proposed. Suitability of AlCs composite at field conditions was tested with a field sample taken from a nearby fluoride-endemic village. This work provides a potential platform for the development of defluoridation technology. (C) 2010 Elsevier B.V. All rights reserved.