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Herein, a porous polymeric carbon nitride (PPCN) with a crystalline backbone was constructed for visible light\u2010induced photocatalytic hydrogen generation by photoexcited electrons, followed by in\u2010situ utilization for olefin hydrogenation. Simultaneously, various alcohols were selectively transformed to valuable aldehydes or ketones by photoexcited holes. The porosity of PPCN provided it with a large surface area and a short transfer path for photogenerated carriers from the bulk to the surface, and the crystalline structure facilitated photogenerated charge transfer and separation, thus enhancing the overall photocatalytic performance. High reactivity and selectivity, good functionality tolerance, and broad reaction scope were achieved by this concerted photocatalysis system. The results contribute to the development of highly efficient semiconductor photocatalysts and synergistic redox reaction systems based on PWST for high\u2010value\u2010added fine chemical production.<\/jats:p>","DOI":"10.1002\/cssc.202101041","type":"journal-article","created":{"date-parts":[[2021,6,27]],"date-time":"2021-06-27T22:21:20Z","timestamp":1624832480000},"page":"3344-3350","update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":25,"title":["Photoredox\u2010Catalyzed Simultaneous Olefin Hydrogenation and Alcohol Oxidation over Crystalline Porous Polymeric Carbon Nitride"],"prefix":"10.1002","volume":"14","author":[{"ORCID":"https:\/\/orcid.org\/0000-0003-2315-4734","authenticated-orcid":false,"given":"Chuntian","family":"Qiu","sequence":"first","affiliation":[{"name":"SZU-NUS Collaborative Center and International Collaborative Laboratory of 2D Materials for Optoelectronic Science &amp; Technology of Ministry of Education Institute of Microscale Optoelectronics Shenzhen University  Shenzhen 518060 P. 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