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This study develops a dual-responsive starch-based conductive hydrogel via a facile \u201cone-pot\u201d strategy, achieving mechanically robust pressure sensing and ultra-sensitive humidity detection. The starch-Poly (2,3-dihydrothieno-1,4-dioxin)-poly (styrenesulfonate) (PEDOT:PSS)-glutaraldehyde (SPG) hydrogel integrates physical entanglement and covalent crosslinking to form a porous dual-network architecture, exhibiting high compressive fracture stress (266 kPa), and stable electromechanical sensitivity (\u0394I\/I0, ~2.3) with rapid response (0.1 s). In its dried state (D-SPG), the film leverages the starch\u2019s hygroscopicity for humidity sensing, detecting minute moisture changes (\u0394RH = 6.6%) within 120 ms and outputting 0.4~0.5 (\u0394I\/I0) signal amplitudes. The distinct state-dependent responsiveness enables tailored applications: SPG monitors physiological motions (e.g., pulse waves and joint movements) via conformal skin attachment, while D-SPG integrated into masks quantifies respiratory intensity with 3\u00d7 signal enhancement during exercise. This work pioneers a sustainable candidate for biodegradable flexible electronics, overcoming trade-off limitations between mechanical integrity, signal stability, and dual responsiveness in starch hydrogels through synergistic network design.<\/jats:p>","DOI":"10.3390\/s25165006","type":"journal-article","created":{"date-parts":[[2025,8,13]],"date-time":"2025-08-13T09:43:01Z","timestamp":1755078181000},"page":"5006","update-policy":"https:\/\/doi.org\/10.3390\/mdpi_crossmark_policy","source":"Crossref","is-referenced-by-count":6,"title":["Dual-Responsive Starch Hydrogels via Physicochemical Crosslinking for Wearable Pressure and Ultra-Sensitive Humidity Sensing"],"prefix":"10.3390","volume":"25","author":[{"given":"Zi","family":"Li","sequence":"first","affiliation":[{"name":"Electronic Information School, Wuhan University, Wuhan 430072, China"},{"name":"Suzhou Institute of Wuhan University, Suzhou 215000, China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jinhui","family":"Zhu","sequence":"additional","affiliation":[{"name":"Electronic Information School, Wuhan University, Wuhan 430072, China"},{"name":"Suzhou Institute of Wuhan University, Suzhou 215000, China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zixuan","family":"Wang","sequence":"additional","affiliation":[{"name":"Electronic Information School, Wuhan University, Wuhan 430072, China"},{"name":"Suzhou Institute of Wuhan University, Suzhou 215000, China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Hao","family":"Hu","sequence":"additional","affiliation":[{"name":"Electronic Information School, Wuhan University, Wuhan 430072, China"},{"name":"Suzhou Institute of Wuhan University, Suzhou 215000, China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-4913-6868","authenticated-orcid":false,"given":"Tian","family":"Zhang","sequence":"additional","affiliation":[{"name":"Electronic Information School, Wuhan University, Wuhan 430072, China"},{"name":"Suzhou Institute of Wuhan University, Suzhou 215000, China"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"1968","published-online":{"date-parts":[[2025,8,13]]},"reference":[{"key":"ref_1","doi-asserted-by":"crossref","unstructured":"Zheng, Q., Xu, C., Jiang, Z., Zhu, M., Chen, C., and Fu, F. 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