Layered double hydroxides (LDH) calcined at different temperatures (denoted as CLDH) have been demonstrated to recover their original layered structure in the presence of appropriate anions. In the light of this so-called "memory effect", a study of removal of fluoride from aqueous solution by calcined Mg-Al-CO3-LDH has been carried out. The LDH calcined at 500 degrees C had the highest capacity of removal of fluoride ion, because of retention of its intrinsic structure. The CLDH with an Mg/Al ratio of 2 has a remarkable ability to adsorb anions. The adsorption loading is higher for the calcined Mg-Al-LDH than for calcined Zn-Al and Ni-Al-LDH. The influence of varying the conditions for removal of fluoride, such as the pH of aqueous solution, the initial fluoride concentration, the dosage of adsorbent, and temperature on removal of fluoride have been investigated. The influence of co-existing anions in fluoride aqueous solution indicates that the percentage of removal of fluoride increased in order PO43- < Cl- approximate to SO42- < Br- << NO3-. It was found that maximum removal of fluoride from aqueous solutions was obtained in 6h at pH 6.0 with an initial concentration of 50 mg/L, and that the retention of fluoride ions by the CLDH material was 98% or higher. The residual fluoride concentration was found to be 0.4 mg/L with an initial concentration of 20 mg/L, which meets the national standard for drinking water quality. The Freundlich isotherm and Langmuir isotherm were used to fit the data of equilibrium experiments. The results of X-ray diffraction, FT-IR and TG-MS demonstrate that the adsorption phenomenon is accompanied by rehydration with concomitant uptake of fluoride ions to rebuild the initial layered structure. (c) 2005 Elsevier B.V. All rights reserved.