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However, creating an efficient pathway for targeted photoelectron transfer at the TM\u2013electrode interface remains challenging. Most studies have focused on extending the electrochemical active area through electrode modification to increase the photocurrent. Here, we establish a redox cascade between TM and the electrode using two newly identified mediators. One mediator is NADP+, the terminal electron acceptor of TM, which is identified for the first time as a natural redox mediator in TM-based bio-solar cells. The other mediator is C60-N,N-dimethyl pyrrolidinium iodide (C60-DMePyI), a water-soluble fullerene derivative that serves as a three-dimensional electron carrier. Given the favorable redox potential alignment between these two mediators, C60-DMePyI functions as a redox helper for NADP+ in the TM-NADP+-C60-DMePyI ternary system. This dual-mediator redox cascade overcomes the kinetic and structural mismatches in interfacial electron transfer, ultimately resulting in an approximately 60-fold enhancement in photocurrent compared to the TM-alone system. This work provides a simple and straightforward strategy to overcome the limited photocurrent of TM by employing dual mediators, opening new possibilities for achieving highly efficient electronic communication between biological membranes and electrodes.<\/jats:p>","DOI":"10.1021\/acsami.6c12970","type":"journal-article","created":{"date-parts":[[2026,10,15]],"date-time":"2026-10-15T11:01:20Z","timestamp":1792062080000},"source":"Crossref","is-referenced-by-count":0,"title":["Dual-Mediator Redox Cascade Enhances Photoelectron Harvesting from Thylakoid Membranes"],"prefix":"10.1021","author":[{"given":"Xuetong","family":"Zhao","sequence":"first","affiliation":[{"name":"University of Science and Technology of China , , ,","place":["Hefei, China, 230027"]},{"name":"Chinese Academy of Sciences , , ,","place":["Beijing, China, 100101"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yanping","family":"Zhang","sequence":"additional","affiliation":[{"name":"Chinese Academy of Sciences , , ,","place":["Beijing, China, 100101"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Linqi","family":"Wang","sequence":"additional","affiliation":[{"name":"Chinese Academy of Sciences , , ,","place":["Beijing, China, 100101"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-0995-3070","authenticated-orcid":true,"given":"Yin","family":"Li","sequence":"additional","affiliation":[{"name":"Chinese Academy of Sciences , , ,","place":["Beijing, China, 100101"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-3198-0596","authenticated-orcid":true,"given":"Huawei","family":"Zhu","sequence":"additional","affiliation":[{"name":"Chinese Academy of Sciences , , ,","place":["Beijing, China, 100101"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,10,15]]},"reference":[{"key":"2026101507011422200_cit1","doi-asserted-by":"publisher","first-page":"4926","DOI":"10.1039\/c9cs00496c","article-title":"Semi-biological approaches to solar-to-chemical conversion","volume":"49","author":"Fang","year":"2020","journal-title":"Chem. 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