Dentine remineralization is clinically significant for prevention and treatment of dentine caries, root caries, and dentine hypersensitivity. However, dentine remineralization is more difficult than enamel remineralization due to the abundant presence of organic matrix in dentine. The objective of this study was to develop a biomimetic method to facilitate remineralization of demineralized dentine through phosphorylation of type I collagen in demineralized dentine using sodium trimetaphosphate. The experimental results indicated that the effect of fluoride on remineralizing dentine was limited when residual mineral crystals were lacking on the surface of demineralized dentine, whereas the phosphorylation and Ca(OH)(2) pretreatment enhanced surface remineralization of the partially demineralized dentine. This biomimetic methodology resulted in favorable surface properties (i.e. highly negative charge and low interfacial free energy between substrate and aqueous medium) for crystal nucleation, and thus could be a promising method to remineralize superficially demineralized dentine lesions.