Provided are compositions comprising theobromine, a source of calcium and a source of phosphate, and methods for preventing dental caries, as well as aqueous compositions and methods for improving the mechanical strength of teeth. Provided in one embodiment is an aqueous composition, said composition comprising: a) isolated theobromine, or a salt or double salt thereof； b) at least one source of calcium, such as calcium chloride, calcium carbonate, calcium gluconate, calcium phosphate, and combinations thereof； c) at least one source of phosphate； and d) a pH of about 5.0 to about 10.0. Optionally further comprising at least one isotonic agent, such as a polyhydric alcohol, such as xylitol, sorbitol, mannitol, maltitol, lactitol, isomalt, erythritol, arabitol, glycerol, and combinations thereof； a thickener, such as methyl cellulose, carboxymethyl cellulose, ethyl cellulose, hydroxypropyl cellulose, and combinations thereof； and an antibacterial agent, such as triclosan, hydrogen peroxide, methyl-4-hydroxybenzoate, clove oil, and combinations thereof.
