It is crucial to emphasize the biomineralization therapeutic method to repair etched dentin in clinic. Non-collagenous proteins (NCPs) play critical role in the biomineralization of dentine. In this paper, we synthesized the phosphate-terminated polyamidoamine dendrimer (PAMAM-PO₃H₂) by one-step modification successfully and examined by Fourier-transform infrared spectroscopy (FTIR) and ¹H-nuclear Magnetic Resonance (¹H-NMR) to characterize the structure of PAMAM-PO₃H₂. PAMAM-PO₃H₂ and carboxylterminated dendrimers (PAMAM-COOH) were applied as the dual biomimetic analogs of NCPs. Through the characterization of FT-IR, field emission scanning electron microscope (FE-SEM), transmission electron microscope (TEM), energy-dispersive X-ray spectroscopy (EDS) and X-ray diffraction (XRD), the surfaces of human dentin were covered with regenerated crystals and the dentinal tubules were occluded by PAMAM-PO₃H₂ and PAMAM-COOH. In summary, the combination of PAMAM-PO₃H₂ and PAMAM-COOH may be another feasible therapeutic method for the treatment of dentin caries and dentin hypersensitivity.