This study investigated carboxymethyl chitosan (CMC)-induced biomimetic mineralization of collagen fibrils, with the aim of synthesizing experimental resins doped with CMC and calcium phosphate microfillers to remineralize artificial caries-affected dentin (ACAD) and enhance resin-dentin bonding durability. A size exclusion test provided evidence for the rejection of CMC (Mw 150 kDa) by collagen fibrils. Transmission electron microscopy and selected area electron diffraction conducted on reconstituted two-dimensional collagen showed typical deposition of needle-like hydroxyapatite crystals within collagen fibrils through CMC-induced biomimetic mineralization. The Vickers hardness test revealed significant improvement (P < 0.001) of the hardness of ACAD treated with CMC-containing experimental resins. Confocal laser scanning microscopy showed reduced dentin permeability and defect sites after biomimetic mineralization. On microtensile bond strength testing, the CMC-remineralized ACAD had better bonding with resin than ACAD and traditionally remineralized ACAD in both self-etch and etch-and-rinse bonding modes (P < 0.001). In conclusion, CMC is efficient in directing the biomimetic mineralization of collagen fibrils. The experimental resins containing CMC can induce dentin biomimetic remineralization and improve the bonding performance of ACAD.
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