LAUSR

The organic–inorganic structure in biological hard tissues ensures their marvelous characteristics but these hybrids are easily destroyed by the demineralization of inorganic components, e.g., the damage of dentin. Current clinical materials for hard tissue regeneration commonly act as “fillers” and their therapeutic effect is limited by the failures of biological‐linked organic–inorganic interface reconstruction. Herein, a fast in situ crosslinking of calcium phosphate oligomers (CPOs) on collagen matrixes for efficient organic–inorganic interface re‐construction, which can result in a biomimetic hybrid, is demonstrated. By using damaged dentin as an example, the inorganic ionic crosslinking can instantly infiltrate into the dentin matrix to rebuild a dense and continuous calcium phosphate‐collagen hybrid within only 5 min, where the structurally integrated organic–inorganic interface is identical to natural dentin. As a result, the damaged dentin can be fully recovered to a healthy one, which is superior to any current dentin treatments. The fast construction of biomimetic hybrid by inorganic ionic crosslinking provides a promising strategy for hard tissue repair and follows great potentials of CPOs as advanced biomedical materials in future.