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The rate of growth of pure calcium fluoride crystals is controlled by a surface polynuclear mechanism when the supersaturation is less than 4.4. The surface free energy is found to be 120 mJ/m2. The dissolution process is also controlled by a surface process. Both of these processes are very strongly inhibited by phosphate ions. Calcium fluoride-like materials contaminated with phosphate are formed when calcium fluoride is precipitated in phosphate-containing solutions or suspensions. The physical and chemical properties of these materials have been investigated and compared with the corresponding properties of pure calcium fluoride. The former dissolve much faster than pure calcium fluoride in solutions containing phosphate, but an inhibitory effect is still shown. It is suggested that the calcium fluoride-like material formed on dental enamel during treatment of enamel with acidified solutions of high fluoride content is a phosphate-containing calcium fluoride.