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Induction of therapeutic angiogenesis represents a promising strategy to restore blood perfusion. Natural bioactive compounds, particularly when integrated with biomaterial engineering, offer therapeutic potential with favorable biosafety profiles. Here, we demonstrate that catalpol (CTP), a bioactive compound from Rehmannia glutinosa, exerts pro-angiogenic effects by enhancing endothelial cell viability, proliferation, migration, and vascular sprouting in vitro. Catalpol upregulates angiogenesis-related markers and promotes angiogenesis via autophagy activation, which is validated using 3-methyladenine (3-MA). To improve local retention and sustained delivery, CTP-loaded silk fibroin nanoparticles (CTP\/SFNP) are self-assembled via mild desolvation and incorporated into gelatin methacryloyl hydrogel (CTP\/SFNP\/GelMA). In a mouse hind limb ischemia model, this hydrogel promotes neovascularization, restores blood perfusion, alleviates tissue injury, and exhibits favorable biocompatibility. These findings highlight the therapeutic potential of CTP\/SFNP\/GelMA for ischemic diseases and identify autophagy activation as a potential mechanism underlying catalpol-mediated angiogenesis, providing insights into nanocarrier design for natural bioactive compounds.<\/jats:p>","DOI":"10.1021\/acsami.6c09967","type":"journal-article","created":{"date-parts":[[2026,10,1]],"date-time":"2026-10-01T20:01:26Z","timestamp":1790884886000},"page":"54414-54431","source":"Crossref","is-referenced-by-count":0,"title":["Catalpol-Loaded Silk Fibroin Nanoparticle\/GelMA Hydrogels Promote Autophagy-Mediated Angiogenesis for Vascular Regeneration in Limb Ischemia"],"prefix":"10.1021","volume":"18","author":[{"ORCID":"https:\/\/orcid.org\/0009-0005-8417-4642","authenticated-orcid":true,"given":"Suya","family":"Chen","sequence":"first","affiliation":[{"name":"Sun Yat-sen University and Guangdong Provincial Key Laboratory of Stomatology , , , ,","place":["Guangzhou, Guangdong, China, 510055"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yuanxiang","family":"Liu","sequence":"additional","affiliation":[{"name":"Sun Yat-sen University and Guangdong Provincial Key Laboratory of Stomatology , , , ,","place":["Guangzhou, Guangdong, China, 510055"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Manjin","family":"Zhang","sequence":"additional","affiliation":[{"name":"Southern Medical University , , , ,","place":["Guangzhou, Guangdong, China, 510260"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yi","family":"Xing","sequence":"additional","affiliation":[{"name":"Southern Medical University , , , ,","place":["Guangzhou, Guangdong, China, 510260"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Liang","family":"Peng","sequence":"additional","affiliation":[{"name":"The First People's Hospital of Guiyang City , , ,","place":["Guiyang, Guizhou, China, 550002"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhen","family":"Zhang","sequence":"additional","affiliation":[{"name":"Southern Medical University , , , ,","place":["Guangzhou, Guangdong, China, 510260"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhipeng","family":"Li","sequence":"additional","affiliation":[{"name":"Sun Yat-sen University and Guangdong Provincial Key Laboratory of Stomatology , , , ,","place":["Guangzhou, Guangdong, China, 510055"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-3341-1485","authenticated-orcid":true,"given":"Zhuofan","family":"Chen","sequence":"additional","affiliation":[{"name":"Sun Yat-sen University and Guangdong Provincial Key Laboratory of Stomatology , , , ,","place":["Guangzhou, Guangdong, China, 510055"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,10,1]]},"reference":[{"issue":"25","key":"2026101404071298500_cit1","doi-asserted-by":"publisher","first-page":"2305","DOI":"10.1056\/NEJMoa2207899","article-title":"Surgery or Endovascular Therapy for Chronic Limb-Threatening Ischemia","volume":"387","author":"Farber","year":"2022","journal-title":"N. 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