The use of organoclays as adsorbents in the remediation of polluted water has been the subject of many recent studies. In the present work, a Tunisian smectite modified with two cationic surfactants was used as an adsorbent to examine the adsorption kinetics, isotherms and thermodynamic parameters of fluoride ions from aqueous solution. Various pH values, initial concentrations and temperatures have been tested. Two simplified kinetic models, first-order and pseudo-second-order, were used to predict the adsorption rate constants. It was found that the adsorption kinetics of fluoride onto modified smectites at different operating conditions can best be described by the pseudo-second-order model. Adsorption isotherms and equilibrium adsorption capacities were determined by the fitting of the experimental data to well known isotherm models including those of Langmuir and Freundlich. The results showed that the Langmuir model appears to fit the adsorption better than the Freundlich adsorption model for the adsorption of fluoride ions onto modified smectites. The equilibrium constants were used to calculate thermodynamic parameters, such as the change of free energy, enthalpy and entropy. Results of this study demonstrated the effectiveness and feasibility of organoclays for the removal of fluoride ions from aqueous solution.