Abstract: Fluoride ions can be removed from an aqueous stream to desirable levels (e.g. less than 1 ppm) using two precipitation reactions in series. In this method, calcium chloride and a phosphate salt are added to form a first precipitate and then a carbonate salt is added to form a second precipitate. However under certain circumstances, the conventional stoichiometries employed have been found to remove insufficient fluoride. Instead, sufficient fluoride can be removed by employing unconventional stoichiometries, specifically excessive calcium chloride or deficient carbonate salt.