Nacre exhibited noticeable similarities in fundamental material buildup and biological characteristics with tooth hard tissue, so the present study aims to achieve bionic dentine remineralization by duplicating nacre's "bottom-up" assembly concept. Inspired by nacre's mineralization mechanism, the present project starts to synthesize a "seawater-like" mineralizing precursor medium, then monitor its in vitro dentinal tubules occlusion effect, acid-resistant stability, the "fingerprint" dynamic components change in real time on in vitro sensitive tooth model as well as its in vitro cellular biological response towards human dental pulp stem cells. For the further exploration, a single-layer fibrillar collagen model was established to simulate the exposed collagen of demineralized dentine to appraise its intrafibrillar mineralization effect. The results demonstrated that the application of "seawater-like" mineralizing precursor medium effectively occluded dentinal tubules, reduced dentine permeability, increased surface microhardness, provided certain acid-resistant stability and possessed favorable in-vitro biocompatibility. In addition, the dynamic procedure of hierarchical intrafibrillar nanocrystalline assembly was observed, which offered a clue to uncover its remineralizing mechanism. It is attainable to realize the biomimetic remineralization of human dentine via the "bottom-up" concept inspired by nacre structure duplication, suggesting great potential for providing dentists a therapeutic strategy to counter dentine hypersensitivity in the future.