Fluoride is an essential component in the mineralization of bones and in the formation of dental enamel. Excessive intake may result, however, in teeth mottling and dental and skeletal fluorosis. With an average fluoride concentration of ~2.4 mg L–1 in Tunisian drinking water, the present study focused on promoting low-cost materials for removal of excess fluoride. Two Tunisian raw clays were used as adsorbents in a batch process to eliminate excess fluoride ions from drinking water and, thus, avoid fluorosis phenomena. Physicochemical characterization and chemical analysis of the raw clays were carried out using X-ray fluorescence, X-ray diffraction, and the BET method. For fluoride removal, the effects of contact time, adsorbent dose, and pH were evaluated. The optimum defluoridation capacity was at 30 min of contact time, 20 g/L of clay dose, and at pH = 3. The kaolinite tested removed more fluoride than smectite. The selected clay was used successfully to remove fluoride from contaminated water with high concentrations of foreign ions that exceeded the potability limits. Adsorption isotherms revealed that the data fitted well to both the Langmuir and Freundlich adsorption isotherms, thus confirming both monolayer and multilayer adsorption.