AbstractCalcium phosphate and bovine serum albumin were coprecipitated (under physiological conditions of temperature and pH) upon the surfaces of titanium‐alloy samples, which thereby became coated with a dense, proteinaceous mineral layer 30–50 μm in thickness. Dissolution of the inorganic phase by treatment with acidic saline yielded a self‐supporting protein scaffold, 7–10 μm in thickness. Energy‐dispersive X‐ray analysis and Fourier‐transform infrared spectroscopy confirmed the absence of inorganic components from the demineralized albumin scaffolds. When titanium‐alloy samples bearing these demineralized protein scaffolds were immersed in a supersaturated solution of calcium phosphate (again at physiological temperature and pH), they remineralized. These redux albumin‐calcium phosphate layers corresponded in thickness to the original coatings. When titanium‐alloy discs bearing the demineralized protein scaffolds were implanted ectopically (subcutaneously) in mice, they, too, remineralized. No uniform mineral layer was deposited upon the surfaces of naked titanium‐alloy implants. To the best of our knowledge, this is the first demonstration of remineralization within the interstices of a noncollagenous protein scaffold, either in vitro or in vivo. © 2003 Wiley Periodicals, Inc. J Biomed Mater Res 67A: 1155–1162, 2003