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Herein, a defect\u2010engineered spatial coupling strategy is devised to construct a heterojunction photocatalyst (Def\u2010CuCN\/NU) by integrating copper single atoms (Cu SA) anchored on polymeric carbon nitride (CN) into the defective NH\n                    <jats:sub>2<\/jats:sub>\n                    \u2010UiO\u201066 (Def\u2010NU). The defective MOFs with porous structure and abundant active sites serve as microreactors that enhance methane adsorption and promote methanol desorption, thus promoting the reaction and minimizing the contact of methanol with \u00b7OH radicals and effectively suppressing overoxidation. Additionally, the heterojunction formed between CuCN and Def\u2010NU accelerates charge separation and transport, which renders efficient photocatalytic conversion of methane to methanol oxygenates. Notably, the Def\u2010CuCN\/NU catalyst affords a high production rate of 1718\u00a0\u00b5mol\u00a0g\n                    <jats:sup>\u22121<\/jats:sup>\n                    \u00a0h\n                    <jats:sup>\u22121<\/jats:sup>\n                    for methanol oxygenates under full\u2010spectrum light irradiation at a remarkable selectivity of 96.5%. This study presents the first demonstration of employing defect\u2010engineered MOFs\u2010based heterojunction photocatalysts for the regulation of the reaction pathway to enable highly selective photocatalytic oxidation of CH\n                    <jats:sub>4<\/jats:sub>\n                    .\n                  <\/jats:p>","DOI":"10.1002\/advs.202513507","type":"journal-article","created":{"date-parts":[[2025,10,28]],"date-time":"2025-10-28T13:23:20Z","timestamp":1761657800000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":3,"title":["Defective MOFs Microreactor with Heterojunction for Selective Methane Photocatalysis via Desorption\u2010Driven Overoxidation Suppression"],"prefix":"10.1002","volume":"13","author":[{"given":"Bo","family":"Feng","sequence":"first","affiliation":[{"name":"Department of Chemistry Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials State Key Laboratory of Porous Materials for Separation and Conversion Fudan University  Shanghai 200438 P. 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