Exploiting efficient and affordable treatment technology for fluoride removal via adsorption isrnhighly desirable. rnIn this study, calcinedhydrotalcites with different Mg/Al molar ratios were prepared. Layeredrndouble hydroxides calcined at 450 have been shown to recover their original layered structurernin the presence of appropriate anions which may enhance its adsorption capacity. Uptake ofrnfluoride ion from aqueous solution by CHT was investigated by batch experiments. The responsernsurface methodology was applied to optimize the adsorption capacity by employing a rnrnfactorial design. The optimal pH, initial fluoride concentration and Mg/Al molar ratio in CHTrnwere found to be 6.0, 5mg/L and 2 respectively for the maximum percentage adsorption ofrn94.4%.The equilibrium isotherm showed that the uptake of fluoride ion by CHT was consistentrnwith the Langmuir and Freundlich equations and that the Langmuir model gave a better fit to thernexperimental data than the Freundlich model. The maximum uptake capacity of CHT for fluoridernion by the Langmuir isotherm model was estimated to be 0.4762 mg/g. The influence of varyingrnpH of solution, initial fluoride concentration and Mg/Al molar ratio in the structure of CHT onrnthe kinetics of fluoride removal has also been explored. Kinetic models were used to fit thernexperimental data, and it was found that the pseudo-second-order kinetics model could be usedrnto describe the uptake process satisfactorily. The present work demonstrates thatrncalcinedhydrotalcites may be promising adsorbents for effective removal of fluorine from waterrnresources.