Safe drinking water is a necessity for every human being, but clean water is scarce and not easily available due to natural geochemical factors or industrial pollutant activity. Many issues involving water quality could be greatly improved using clays as adsorbents. We highlight for the first time, the uptake of fluoride from natural water by Laponite, synthetic hectorite clay, in raw and modified state. A series of batch adsorption experiments were carried out to evaluate the adsorption potential of the different parameters. The optimized parameters were: contact time, adsorbent dose and pH. It was found that fluoride uptake from natural water was better using raw Laponite and inorganic-modified Laponite than using organic-modified Laponite clays. Adsorbents were characterized before and after fluoride adsorption by X-ray diffraction, X-ray fluorescence, FTIR, thermo gravimetric analyses and 19F solid state NMR spectroscopy. The experimental data showed that both Langmuir and Freundlich models fitted an adsorption isotherm well. Thermodynamic parameters such as Gibbs free energy (ΔG°), enthalpy (ΔH°), and entropy (ΔS°) were calculated. These parameters indicated that fluoride adsorption onto Laponite was nonspontaneous and endothermic in temperature range between 25 and 45 °C.