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The ubiquitous moisture and sunlight in nature are attractive for sustainable power generation especially. A high\u2010performance light\u2010coordinated \u201cmoist\u2010electric generator\u201d (LMEG) based on the rational combination of a polyelectrolyte and a phytochrome is herein developed. By spontaneous adsorption of gaseous water molecules and simultaneous exposure to sunlight, a piece of 1 cm<jats:sup>2<\/jats:sup> composite film offers an open\u2010circuit voltage of 0.92\u00a0V and a considerable short\u2010circuit current density of up to 1.55\u00a0mA cm<jats:sup>\u22122<\/jats:sup>. This record\u2010high current density is about two orders of magnitude improvement over that of most conventional moisture\u2010enabled systems, which is caused by moisture\u2010induced charge separation accompanied with photoexcited carrier migration, as confirmed by a dynamic Monte Carlo device simulation. Flexible devices with customizable size are available for large\u2010scale integration to effectively work under a wide range of relative humidity (about 20\u2013100%), temperature (10\u201380\u00a0\u00b0C), and light intensity (30\u2013200\u00a0mW cm<jats:sup>\u22122<\/jats:sup>). The wearable and portable LMEGs provide ample power supply in natural conditions for indoor and outdoor electricity\u2010consuming systems. This work opens a novel avenue to develop sustainable power generation through collecting multiple types of natural energy by a single hybrid harvester.<\/jats:p>","DOI":"10.1002\/adma.202103897","type":"journal-article","created":{"date-parts":[[2021,12,29]],"date-time":"2021-12-29T16:18:19Z","timestamp":1640794699000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":142,"title":["Sunlight\u2010Coordinated High\u2010Performance Moisture Power in Natural Conditions"],"prefix":"10.1002","volume":"34","author":[{"given":"Jiaxin","family":"Bai","sequence":"first","affiliation":[{"name":"State Key Laboratory of Tribology Department of Mechanical Engineering Tsinghua University  Beijing 100084 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yaxin","family":"Huang","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Tribology Department of Mechanical Engineering Tsinghua University  Beijing 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