Abstract: Provided herein are novel compositions for the restoration of demineralized tissues, such as dentin which has been demineralized by tooth decay. The remineralization agent comprises a bioactive ceramic component and a polyanionic macromolecular component, which may be admixed and applied to the target tissue and which will subsequently set to produce a remineralizing solid. The remineralizing solid will produce nanodroplets of mineral precursor solution, which such nanodroplets can infiltrate demineralized collagen matrices and which will form hydroxyapatite crystals therein by polymer-induced liquid precursor processes. The scope of the invention encompasses novel compositions and methods of treating demineralized tissues.