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Organic photocatalysis can effect metal\u2010free oxidase chemistry. Nevertheless, current methods are limited in reaction scope, possibly due to the lack of suitable photocatalysts. Here we report an isoquinoline\u2010derived diaryl ketone\u2010type photocatalyst, which has much enhanced absorption of blue and visible light compared to conventional diaryl ketones. This photocatalyst enables dehydrogenative cross\u2010coupling of heteroarenes with unactivated and activated alkanes as well as aldehydes using air as the oxidant. A wide range of heterocycles with various functional groups are suitable substrates. Transient absorption and excited\u2010state quenching experiments point to an unconventional mechanism that involves an excited state \u201cself\u2010quenching\u201d process to generate the N\u2010radical cation form of the sensitizer, which subsequently abstracts a hydrogen atom from the alkane substrate to yield a reactive alkyl radical.\n                  <\/jats:p>","DOI":"10.1002\/anie.202202649","type":"journal-article","created":{"date-parts":[[2022,3,7]],"date-time":"2022-03-07T05:37:48Z","timestamp":1646631468000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":25,"title":["Oxidase\u2010Type C\u2212H\/C\u2212H Coupling Using an Isoquinoline\u2010Derived Organic Photocatalyst"],"prefix":"10.1002","volume":"61","author":[{"given":"Lei","family":"Zhang","sequence":"first","affiliation":[{"name":"Laboratory of Inorganic Synthesis and Catalysis Institute of Chemical Sciences and Engineering \u00c9cole Polytechnique 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