Mouth rinses, dentifrices, lozenges, confections, chewing gums, and similar delivery vehicles containing non-toxic soluble calcium are used prior to administration of a fluoride-containing composition to increase the effectiveness of the fluoride therapy. An effective amount of calcium is released into the oral cavity and allowed to penetrate into the oral tissue. Calcium-bound fluoride deposits form in the oral tissue upon subsequent administration of the fluoride-containing composition to provide increased salivary, plaque and oral tissue fluoride concentrations.