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Here, n\u2010type giant\u2010molecule\u2010type organic semiconductors GSY\u2010C4 and GSY\u2010C10 with tailored alkyl chains were developed for waterproof organic photodetectors (OPDs). D18:GSY\u2010C4 and D18:GSY\u2010C10 bulk heterojunctions enabled stable underwater photoplethysmography sensing, with peak responsivities of \u223c1.31 and \u223c0.7 A W\n                    <jats:sup>\u22121<\/jats:sup>\n                    , respectively. Short\u2010term water exposure did not cause obvious irreversible degradation, but induced water\u2010triggered adaptive structural reorganization, supported by reduced lamellar d\u2010spacing, increased lamellar coherence length, and preserved \u03c0\u2013\u03c0 stacking. After 4\u00a0h water immersion, unencapsulated D18:GSY\u2010C4 arrays (\n                    <jats:italic>n<\/jats:italic>\n                    = 49) showed a \u223c9% reduction in dark\u2010current density and nearly unchanged responsivity (\n                    <jats:italic>\n                      R\n                      <jats:sub>\u03bb<\/jats:sub>\n                    <\/jats:italic>\n                    ) and specific detectivity (\n                    <jats:italic>D<\/jats:italic>\n                    *). Moreover, key current parameters could be recovered through ethanol rinsing and mild annealing at 100\u00b0C for 20\u00a0min. D18:GSY\u2010C10 OPDs maintained underwater functionality for 9 days with &lt;10% variation in dark\u2010 and photocurrent densities, highlighting alkyl\u2010chain engineering as an effective strategy for aqueous\u2010stable organic optoelectronics.\n                  <\/jats:p>","DOI":"10.1002\/adma.74922","type":"journal-article","created":{"date-parts":[[2026,9,12]],"date-time":"2026-09-12T03:21:01Z","timestamp":1789183261000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Unencapsulated Self\u2010Hydroadaptive Organic Heterojunctions for Underwater Physiological Monitoring"],"prefix":"10.1002","author":[{"given":"Tingting","family":"Yan","sequence":"first","affiliation":[{"name":"College of Smart Materials and Future Energy State Key Laboratory of Molecular Engineering of Polymers Fudan University  Shanghai P. R. 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