Calcium peroxyphosphate compounds and dental compositions comprising these compounds that combine both whitening/stain removal of teeth with remineralization are disclosed. The calcium peroxyphosphate compounds are capable of releasing, in an aqueous environment, whitening and remineralization effective amounts of calcium ion, phosphate ion, and active oxygen. Preferred compounds are calcium peroxymonophosphate or calcium diperoxymonophosphate compounds. These compounds may be used in humans and other animals, including other mammals.