The experiments showed that a part of the fluoride which was taken up by hydroxyapatite or teeth at low concentrations of fluoride at neutral pH was soluble in alkali (IN KOH, 24 h) and was thus not fluoroapatite. Calcium fluoride could not form under the present conditions because the solubility of this compound was not exceeded. It is suggested that the alkali soluble fluoride is adsorbed to calcium ions bound as counterions in the hydration layer of the hydroxyapatite or the enamel. This is consistent with previous findings in this laboratory, showing that fluoride displaced acidic proteins adsorbed to calcium receptors on the hydroxyapatite surface in the same way as other anions displace proteins.It could also be shown that polyanions and polycations adsorbed to hydroxyapatite surfaces by ionic exchange, displacing phosphate or phosphate and calcium respectively in the process. A model is suggested which differs slightly from that proposed by Bernardi.