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Poly(vinylphosphonic acid) (PVPA) and sodium trimetaphosphate (STMP) as templating analogs of NCPs induce hierarchical mineralization in cooperation with indispensable sequestration analogs such as polyacrylic acid (PAA) via polymer\u2010induced liquid\u2010like precursor (PILP) process. Herein, STMP\u2010Ca and PVPA\u2010Ca complexes are proposed to achieve rapid intrafibrillar mineralization through polyelectrolyte\u2010Ca complexes pre\u2010precursor (PCCP) process. This strategy is further verified effectively for remineralization of demineralized dentin matrix both in vitro and in vivo. Although STMP micromolecule fails to stabilize amorphous calcium phosphate (ACP) precursor, STMP\u2010Ca complexes facilely permeate into intrafibrillar interstices and trigger phase transition of ACP to hydroxyapatite within collagen. In contrast, PVPA\u2010stabilized ACP precursors lack liquid\u2010like characteristic and crystallize outside collagen due to rigid conformation of PVPA macromolecule, while PVPA\u2010Ca complexes infiltrate into partial intrafibrillar intervals under electrostatic attraction and osmotic pressure as evidenced by intuitionistic 3D stochastic optical reconstruction microscopy (3D\u2010STORM). The study not only extends the variety and size range of polyelectrolyte for PCCP process but also sheds light on the role of phosphorylation for NCPs in biomineralization.<\/jats:p>","DOI":"10.1002\/adhm.202400102","type":"journal-article","created":{"date-parts":[[2024,4,24]],"date-time":"2024-04-24T15:38:55Z","timestamp":1713973135000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":13,"title":["STMP and PVPA as Templating Analogs of Noncollagenous Proteins Induce Intrafibrillar Mineralization of Type I Collagen via PCCP Process"],"prefix":"10.1002","volume":"13","author":[{"ORCID":"https:\/\/orcid.org\/0000-0001-6653-4310","authenticated-orcid":false,"given":"Yiru","family":"Wang","sequence":"first","affiliation":[{"name":"Stomatology Hospital School of Stomatology Zhejiang University School of Medicine Zhejiang Provincial Clinical Research Center for Oral Diseases Key Laboratory of Oral Biomedical Research of Zhejiang 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