Magnesium, nickel, and cobalt hydrotalcite-like compounds (MgAlHT, NiAlHT, and CoAlHT) were used to remove fluoride ions from aqueous solutions and drinking water in batch and column systems. Mg, Ni, and Co hydrotalcite like compounds with similar M2+:Al3+ ratios were synthesized. F- ions were determined in the remaining solutions using a fluoride ion selective electrode. Kinetic of the fluoride sorption from aqueous solutions by hydrotalcite-like compounds (HT) was best described by the pseudo-second-order model and the equilibrium was reached in less than 200 minutes for all cases (MgAlHT, NiAlHT and CoAlHT); however, this behavior was not observed for fluoride sorption from drinking water by NiAlHT. The sorption isotherms of the fluoride ion by hydrotalcite like compounds could be best fitted to the Langmuir and Freundlich models. NiAlHT showed the highest efficiency for the removal of fluoride ions from aqueous solutions in batch system. The removal of fluoride ions by NiAlHT from aqueous solutions was more efficient than from drinking water in both batch and column systems.