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While starch\u2010based hydrogels present a promising sustainable alternative, their widespread application is limited by inherent brittleness and significant signal hysteresis. Here, a molecular engineering strategy is proposed to address these limitations. Porous starch is first obtained through a gradual solvent exchange process to enhance chain accessibility. Protocatechuic acid (PCA) is then covalently grafted onto the starch backbone via EDC\/NHS\u2010mediated esterification, introducing dynamic hydrogen\u2010bonding and \u03c0 \u2212 \u03c0 interaction motifs. By optimizing the ratio between PCA\u2010modified starch and polyacrylamide (PAM), a bioinspired hydrogel with exceptional toughness and rapid electromechanical response is achieved. The resultant hydrogel exhibited pronounced strain\u2010dependent resistance behavior, enabling its integration into a wireless wearable human\u2010machine interface. To ensure robust decoding against motion\u2010induced noise, a finite state machine (FSM)\u2010based algorithm is employed for adaptive signal segmentation, achieving a character\u2010level accuracy of 99.2% in trials with healthy subjects (\n                    <jats:italic>n<\/jats:italic>\n                    = 10). This work not only introduces a high\u2010performance, sustainable hydrogel platform but also demonstrates a practical route toward inclusive and language\u2010independent human\u2010machine communication.\n                  <\/jats:p>","DOI":"10.1002\/smll.202514890","type":"journal-article","created":{"date-parts":[[2026,1,29]],"date-time":"2026-01-29T08:18:21Z","timestamp":1769674701000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":6,"title":["Bioinspired Ultratough and Rapidly Responsive Hydrogels Empower Silent Communication"],"prefix":"10.1002","volume":"22","author":[{"given":"Shuaibo","family":"Zhang","sequence":"first","affiliation":[{"name":"Hubei Engineering Technology Research Center of Spectrum and Imaging Instrument Electronic Information School Wuhan University No. 299, Bayi Road, Wuchang District Wuhan P. R. China"},{"name":"Wuhan Institute of Quantum Technology Wuhan P. R. 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