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Herein, we report an inverse-structured MgO\/Co catalyst featuring highly dispersed MgO nano-islands on metallic Co nanoparticles, which effectively overcomes these limitations. Under illumination at 2.33 W\u00b7cm\u20132 without external heating, the optimized 5MgO\/Co catalyst achieves a remarkable CH4 production rate of 458 mmol\u00b7gcat\u20131\u00b7h\u20131 with a CH4 selectivity of 98.5%, outperforming most non-noble-metal and several noble-metal benchmarks. Furthermore, the inverse catalyst demonstrates outstanding durability, maintaining stable performance over 50 hours with robust coking resistance. In situ spectroscopic studies and theoretical calculations reveal that the inverse MgO\/Co interface regulates the adsorption configuration of formate intermediates, thereby accelerating their subsequent hydrogenation toward CH4. Meanwhile, plasmonic Co nanoparticles promote efficient photothermal conversion and interfacial charge transfer, facilitating CO2 activation and H2 dissociation at the oxide\u2013metal boundary. This synergistic coupling of inverse-interface catalysis, localized photothermal heating, and photoinduced electron transfer enables highly efficient solar-driven CO2 methanation, establishing inverse MgO\/Co as a powerful platform for robust and selective CO2 upgrading.<\/jats:p>","DOI":"10.1021\/acsami.6c13368","type":"journal-article","created":{"date-parts":[[2026,9,10]],"date-time":"2026-09-10T22:01:29Z","timestamp":1789077689000},"page":"50978-50990","source":"Crossref","is-referenced-by-count":0,"title":["Inverse MgO\u2013on\u2013Co Interfaces Enable Highly Efficient and Stable Photothermal CO2 Methanation via Regulation of Key Intermediate Conversion"],"prefix":"10.1021","volume":"18","author":[{"given":"Yousheng","family":"Cao","sequence":"first","affiliation":[{"name":"Tianjin University , , ,","place":["Tianjin, China, 300072"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xu","family":"Hu","sequence":"additional","affiliation":[{"name":"Tianjin University , , ,","place":["Tianjin, China, 300072"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-5872-8502","authenticated-orcid":true,"given":"Xusheng","family":"Wang","sequence":"additional","affiliation":[{"name":"Zhejiang Sci-Tech University , , ,","place":["Hangzhou, China, 310018"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-6773-8769","authenticated-orcid":true,"given":"Hongwei","family":"Zhang","sequence":"additional","affiliation":[{"name":"Biogas Institute of Ministry of Agriculture and Rural Affairs , , ,","place":["Chengdu, China, 610041"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-9273-2898","authenticated-orcid":true,"given":"Haijiao","family":"Lu","sequence":"additional","affiliation":[{"name":"The University of Queensland , , , QLD ,","place":["St Lucia, Australia, 4072"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-8105-8903","authenticated-orcid":true,"given":"Jinhua","family":"Ye","sequence":"additional","affiliation":[{"name":"Tianjin University , , ,","place":["Tianjin, China, 300072"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-6424-7959","authenticated-orcid":true,"given":"Hui","family":"Song","sequence":"additional","affiliation":[{"name":"Tianjin University , , ,","place":["Tianjin, China, 300072"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,9,10]]},"reference":[{"key":"2026102013063010400_cit1","doi-asserted-by":"publisher","first-page":"3169","DOI":"10.1038\/s41467-019-10996-2","article-title":"Fundamentals and applications of photocatalytic CO2 methanation","volume":"10","author":"Ulmer","year":"2019","journal-title":"Nat. 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