Remineralized dentin with an antibacterial ability is still a significant challenge in dentistry. Previously, a polyelectrolyte‐calcium complexes pre‐precursor (PCCP) process is proposed for rapid collagen mineralization. In the present study, the expansion concept of the PCCP process is explored by replacing the calcium with other cations, such as strontium. The results of transmission electron microscopy (TEM), 3D stochastic optical reconstruction microscopy, energy‐dispersive X‐ray analysis, Fourier transform infrared spectroscopy, and high‐resolution TEM with selected area electron diffraction demonstrate that biomimetic mineralization of collagen fibrils and demineralized dentin could be fulfilled with Sr&F‐codoped hydroxyapatite (HAp) after they are treated with poly‐aspartic acid‐strontium (PAsp‐Sr) suspension followed by a phosphate&fluoride solution. Moreover, dentin remineralized with Sr&F‐codoped HAp exhibits in vitro and in vivo antibacterial ability against Streptococcus mutans. The cytotoxicity and oral mucosa irritation tests reveal excellent biocompatibility of mineralization mediums (PAsp‐Sr suspension and phosphate&fluoride solution). The demineralized dentin's mechanical properties (elastic modulus and microhardness) could be restored almost to that of the intact dentin. Hence, the expansion concept of the PCCP process that replaces calcium ions with some cationic ions along with fluorine opens up new horizons for generating antibacterial remineralized dentin containing ions‐doped HAp with excellent biocompatibility via biomimetic mineralization technology.