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However, the in situ (post\u2010injection) fabrication of abundant porous structures permissive for cellular ingrowth\u2014a fundamental requirement for achieving efficient bone regeneration\u2014poses a considerable challenge. Here, this study finds that calcium polyphosphate (Ca\u2010polyP) coacervate, a liquid precursor of osteogenic Ca\u2010polyP solid, enables in situ dual pore\u2010forming individually or simultaneously: setting\u2010induced liquid\u2013solid phase separation (SIPS) and setting\u2010induced gas foaming (SIGF), which can be triggered by different inorganic base substances as setting initiators. Notably, SIPS pioneers the observation of such a process in inorganic self\u2010setting systems. Following this, we develop an array of injectable and self\u2010setting Ca\u2010polyP coacervate\u2010based composites, where the two mechanisms produce distinct pore size ranges in situ, i.e., tens\u2010micrometers via SIPS and hundreds\u2010micrometers via SIGF. Variable setting initiators allow tuning of composition and properties. We further apply a typical composite (IS\u2010polyP) with in situ formed hierarchical pores built upon simultaneous SIPS and SIGF for bone repair. Investigations reveal that IS\u2010polyP can significantly enhance energy metabolism, cell proliferation, and osteogenic differentiation of BMSCs, ultimately promoting bone regeneration and growth of new bone in the macropores. This work establishes a universal design strategy for in situ porous implants in orthopedics.<\/jats:p>","DOI":"10.1002\/smll.76367","type":"journal-article","created":{"date-parts":[[2026,10,23]],"date-time":"2026-10-23T14:30:22Z","timestamp":1792765822000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Setting\u2010Induced Dual Pore Formation in Polyphosphate Coacervate Enables Injectable Implants With In Situ Hierarchical Porosity and Tunable Compositions for Bone Regeneration"],"prefix":"10.1002","author":[{"ORCID":"https:\/\/orcid.org\/0000-0003-2289-4669","authenticated-orcid":false,"given":"Hua","family":"Zeng","sequence":"first","affiliation":[{"name":"Center for Orthopedic Science and Translational Medicine Department of Orthopedics Shanghai Tenth People's Hospital School of Medicine Tongji University  Shanghai China"},{"name":"Shanghai Key Laboratory of Craniomaxillofacial Development and Diseases Shanghai Stomatological Hospital &amp; School of Stomatology Fudan University  Shanghai China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xiong","family":"Luo","sequence":"additional","affiliation":[{"name":"Department of Joint and Sports Medicine Shanghai Fourth People's Hospital School of Medicine Tongji University  Shanghai China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-1343-2761","authenticated-orcid":false,"given":"Ming","family":"Shen","sequence":"additional","affiliation":[{"name":"Shanghai Key Laboratory of Magnetic Resonance Institute of Magnetic Resonance and Molecular Imaging in Medicine School of Physics and Electronic Science East China Normal University  Shanghai China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Rui","family":"Xu","sequence":"additional","affiliation":[{"name":"Center for Orthopedic Science and Translational Medicine Department of Orthopedics Shanghai Tenth People's Hospital School of Medicine Tongji University  Shanghai China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7239-7877","authenticated-orcid":false,"given":"Shuo","family":"Tan","sequence":"additional","affiliation":[{"name":"Center for Orthopedic Science and Translational Medicine Department of Orthopedics Shanghai Tenth People's Hospital School of Medicine Tongji University  Shanghai China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhangling","family":"Nie","sequence":"additional","affiliation":[{"name":"Shanghai Key Laboratory of Craniomaxillofacial Development and Diseases Shanghai Stomatological Hospital &amp; School of Stomatology Fudan University  Shanghai China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Wei","family":"Huang","sequence":"additional","affiliation":[{"name":"Shanghai Key Laboratory of Craniomaxillofacial Development and Diseases Shanghai Stomatological Hospital &amp; School of Stomatology Fudan University  Shanghai China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yali","family":"Han","sequence":"additional","affiliation":[{"name":"Shanghai Key Laboratory of Craniomaxillofacial Development and Diseases Shanghai Stomatological Hospital &amp; School of Stomatology Fudan University  Shanghai China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7327-457X","authenticated-orcid":false,"given":"Xiaoling","family":"Wei","sequence":"additional","affiliation":[{"name":"Shanghai Key Laboratory of Craniomaxillofacial Development and Diseases Shanghai Stomatological Hospital &amp; School of Stomatology Fudan University  Shanghai China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7856-8091","authenticated-orcid":false,"given":"Mei","family":"Li","sequence":"additional","affiliation":[{"name":"Department of Oral Sciences Faculty of Dentistry University of Otago  Dunedin New Zealand"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-2427-2812","authenticated-orcid":false,"given":"Zhaoyong","family":"Zou","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Advanced Technology for Material Synthesis and Processing Wuhan University of Technology  Wuhan China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-1162-1684","authenticated-orcid":false,"given":"Feng","family":"Chen","sequence":"additional","affiliation":[{"name":"Shanghai Key Laboratory of Craniomaxillofacial Development and Diseases Shanghai Stomatological Hospital &amp; 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