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Herein, we report a solvent\u2010vapor spin\u2010coating (SVS) strategy combining chloroform:methanol mixed solutions, which simultaneously induces a shallow island\u2010like surface modulation and optimizes molecular packing. The former improves light harvesting and reduces angular sensitivity, whereas the latter contributes to improved optoelectronic performance; together, they are also associated with enhanced mechanical flexibility. Consequently, organic photovoltaics (OPVs) based on this strategy achieve a power conversion efficiency (PCE) of 20.28% on rigid substrates; more importantly, ultra\u2010flexible devices exhibit a record PCE of 19.03%, accompanied by improved mechanical robustness and reduced angular sensitivity. For organic photodetectors (OPDs), the enhanced light\u2010harvesting translates to a high specific detectivity (\n                    <jats:italic>D<\/jats:italic>\n                    *) exceeding 10\n                    <jats:sup>13<\/jats:sup>\n                    Jones across the 320\u2013920\u00a0nm range, and a response time of &lt; 10 \u00b5s. Finally, for the first time, we demonstrate a top\u2010illumination\/top\u2010emission ultra\u2010flexible photoplethysmography (PPG) sensor by integrating an OPV module, an organic light\u2010emitting diode (OLED), and an OPD, which accurately records on\u2010skin pulse signals. This study provides a promising route to co\u2010optimize the power output, detection sensitivity, and mechanical ductility of organic optoelectronics for practical applications.\n                  <\/jats:p>","DOI":"10.1002\/adma.74032","type":"journal-article","created":{"date-parts":[[2026,7,8]],"date-time":"2026-07-08T22:55:07Z","timestamp":1783551307000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Synergistically Enhancing Light Harvesting and Mechanical Flexibility for Ultra\u2010Flexible Organic Biosensors"],"prefix":"10.1002","volume":"38","author":[{"given":"Xiangjun","family":"Zheng","sequence":"first","affiliation":[{"name":"State Key Laboratory of Silicon and Advanced Semiconductor Materials MOE Key Laboratory of Macromolecular Synthesis and Functionalization Department of Polymer Science and Engineering Zhejiang University  Hangzhou P. R. 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