Bioinspired mineral-in-shell nanoarchitectonics: Functional empowerment of mineral precursors for guiding intradentinal mineralization

Effective mineralization of biological structures poses a significant challenge in hard tissue engineering as it necessitates overcoming geometric complexities and multistep biomineralization processes. In this regard, we propose “mineral-in-shell nanoarchitectonics”, inspired by the nanostructure of matrix vesicles, which can influence multiple mineralization pathways. Our nanostructural design empowers mineral precursors with tailorable properties through encapsulating amorphous calcium phosphate within a multifunctional tannic acid (TA) and silk fibroin (SF) nanoshell. The bioinspired nanosystem facilitates efficient recruitment of mineral precursors throughout the dentin structures, followed by large-scale intradentinal mineralization both in vitro and in vivo , which provides persistent protection against external stimuli. Theoretical simulations combined with experimental studies attribute the success of intradentinal mineralization to the TA-SF nanoshell, which exhibits a strong affinity for the dentin structure, stabilizing amorphous precursors and thereby facilitating concomitant mineral formation. Overall, this bioinspired mineral-in-shell nanoarchitectonics shows a promising prospect for hard tissue repair and serves as a blueprint for next-generation biomineralization-associated materials.