A novel alginate-montmorillonite biopolymer-clay composite bead formulation for water defluoridation was developed in this study. Montmorillonite was dispersed alginate solution, and the mixture was cross-linked in an aqueous solution of aluminum(III). The resulting cross-linked beads were characterized using FTIR, SEM, and mechanical measurements. In order to reveal the defluoridation capacity of the beads, batch adsorption experiments were carried out. Optimum conditions and effect of competing ions were investigated. Experimental data were modeled using several isothermal, kinetic, and thermodynamic models. Maximum Langmuir adsorption capacity was reached as 31.0 mg g(-1) at 25 degrees C. It is also found that the adsorption is physical in nature and follows the Elovich kinetic model, and the fluoride removal efficiency is not affected by the presence of most competing anions. The results show that aluminum alginate-montmorillonite composite beads can be used as effective and natural sorbents for fluoride removal from water.