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Here, we report a rationally designed calcium-aluminosilicate dendritic mesoporous silica nanoparticle (CaAl-DMSN) that integrates heterogeneous catalytic growth factor activation with pro-coagulant and osteogenic functionalities in a single nanoscale platform. Featuring a four-coordinate aluminosilicate framework functionalized with calcium in a radial large-pore architecture, CaAl-DMSN generates a nanoconfined alkaline microenvironment via Ca2+ mediated hydroxide enrichment. This enables more than an order-of-magnitude higher activation efficiency of latent Transforming Growth Factor \u03b21 (TGF-\u03b21) compared to conventional homogeneous alkaline catalysis. Molecular dynamics simulations reveal a markedly reduced free-energy barrier for TGF-\u03b21 dissociation, establishing a direct structure\u2013function relationship between composition, nanostructure, and catalytic activity. Functionally, CaAl-DMSN induces rapid clot formation, enhances CD105+ CD73+ mesenchymal stromal cell recruitment, and promotes osteogenic differentiation via Smad signaling activation. In a rat critical-size calvarial defect model, CaAl-DMSN increases bone volume fraction by \u223c80% compared with controls, while exhibiting excellent biocompatibility. Collectively, CaAl-DMSN couples interfacial chemistry, endogenous growth factor activation, hemostasis, and regenerative microenvironment modulation, offering a growth factor-free strategy for bone repair and broader tissue regeneration applications.<\/jats:p>","DOI":"10.1021\/acsnano.6c05126","type":"journal-article","created":{"date-parts":[[2026,9,3]],"date-time":"2026-09-03T19:30:02Z","timestamp":1788463802000},"page":"24656-24670","source":"Crossref","is-referenced-by-count":0,"title":["Multifunctional\nMesoporous Calcium-Aluminosilicate\nNanoparticles Enable Heterogeneous Activation of Endogenous Transforming\nGrowth Factor \u03b21 and Rapid Hemostasis for Bone Repair"],"prefix":"10.1021","volume":"20","author":[{"ORCID":"https:\/\/orcid.org\/0000-0001-8831-3607","authenticated-orcid":true,"given":"Chun","family":"Xu","sequence":"first","affiliation":[{"name":"The University of Sydney , , , ,","place":["Sydney, New South Wales, Australia, 2006"]},{"name":"The University of Sydney 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2006"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Juan","family":"Wen","sequence":"additional","affiliation":[{"name":"The University of Queensland , , , ,","place":["Brisbane, Queensland, Australia, 4006"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yiwei","family":"Li","sequence":"additional","affiliation":[{"name":"The University of Sydney , , , ,","place":["Camperdown, New South Wales, Australia, 2006"]},{"name":"The University of Sydney , , , ,","place":["Sydney, New South Wales, Australia, 2006"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Huan","family":"Dai","sequence":"additional","affiliation":[{"name":"The University of Queensland , , , ,","place":["Brisbane, Queensland, Australia, 4006"]},{"name":"The University of Queensland , , , ,","place":["St Lucia, Queensland, Australia, 4072"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Siyuan","family":"Liu","sequence":"additional","affiliation":[{"name":"The University of Sydney , , , ,","place":["Sydney, New South Wales, Australia, 2006"]},{"name":"The University of Sydney , , , ,","place":["Camperdown, New South Wales, Australia, 2006"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Dan","family":"Cheng","sequence":"additional","affiliation":[{"name":"The University of Queensland , , , ,","place":["St Lucia, Queensland, Australia, 4072"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yaping","family":"Song","sequence":"additional","affiliation":[{"name":"The University of Queensland , , , ,","place":["St Lucia, Queensland, Australia, 4072"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Bing","family":"Sun","sequence":"additional","affiliation":[{"name":"The University of Queensland , , , ,","place":["St Lucia, Queensland, Australia, 4072"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jie","family":"Tang","sequence":"additional","affiliation":[{"name":"The University of Queensland , , , ,","place":["St Lucia, Queensland, Australia, 4072"]},{"name":"Monash University , , , ,","place":["Melbourne, Victoria, Australia, 3052"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-8380-6338","authenticated-orcid":true,"given":"Jie","family":"Fan","sequence":"additional","affiliation":[{"name":"Zhejiang University , , ,","place":["Hangzhou, China, 310027"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Chang","family":"Lei","sequence":"additional","affiliation":[{"name":"The University of Sydney , , , ,","place":["Camperdown, New South Wales, Australia, 2006"]},{"name":"The University of Sydney , , , ,","place":["Sydney, New South Wales, Australia, 2006"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-3707-0785","authenticated-orcid":true,"given":"Chengzhong","family":"Yu","sequence":"additional","affiliation":[{"name":"The University of Queensland , , , ,","place":["St Lucia, Queensland, Australia, 4072"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,9,3]]},"reference":[{"key":"2026091510072249500_cit1","doi-asserted-by":"publisher","first-page":"103282","DOI":"10.1016\/j.mtbio.2026.103282","article-title":"From bone replacement\nto regeneration. 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