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Herein, a metal\u2013organic framework (MOF)-templated precursor strategy is employed to regulate the initial spatial distribution of Cu and In species, thereby generating Cu\/In2O3 catalysts with distinct MSI regimes. Among the three MSI regimes constructed, the MIL-68(In)-derived catalyst exhibits a moderated MSI that provides a favorable balance between interfacial activation and structural stability. The MOF-derived catalyst suppresses Cu\u2013In alloy formation while promoting oxygen-vacancy generation and maintaining a balanced Cu0\/Cu\u03b4+ equilibrium. The MIL-derived catalyst achieves a methanol space\u2013time yield of 0.374 gMeOH\u00b7gcat\u20131\u00b7h\u20131 at 300 \u00b0C with stable performance. In situ DRIFTS measurements indicate that moderated MSI accelerates the conversion of formate intermediates into methoxy species, while DFT calculations provide atomistic insight into MSI-dependent interfacial charge transfer and H2\/CO2 adsorption. In contrast, excessively strong MSI drives irreversible Cu\u2013In alloy formation, whereas weak MSI leads to insufficient interfacial activation and particle sintering. These findings establish an optimal MSI regime for balancing interfacial reactivity and structural durability and highlight MOF-templated precursor engineering as an effective strategy for designing robust Cu\/In2O3 catalysts for CO2 hydrogenation.<\/jats:p>","DOI":"10.1021\/acsami.6c11826","type":"journal-article","created":{"date-parts":[[2026,8,4]],"date-time":"2026-08-04T13:22:25Z","timestamp":1785849745000},"page":"42757-42768","source":"Crossref","is-referenced-by-count":0,"title":["Establishing an Optimal Metal\u2013Support Interaction Regime in Cu\/In2O3 Catalysts for Stable CO2 Hydrogenation to Methanol"],"prefix":"10.1021","volume":"18","author":[{"given":"Zepu","family":"Jin","sequence":"first","affiliation":[{"name":"Tianjin University , , ,","place":["Tianjin, China, 300072"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Junxin","family":"Guo","sequence":"additional","affiliation":[{"name":"Tianjin University , , ,","place":["Tianjin, China, 300072"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jiawen","family":"Chen","sequence":"additional","affiliation":[{"name":"Tianjin University , , ,","place":["Tianjin, China, 300072"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0005-8697-589X","authenticated-orcid":true,"given":"Anyu","family":"Zhang","sequence":"additional","affiliation":[{"name":"Tianjin University , , ,","place":["Tianjin, China, 300072"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Dule","family":"Huhe","sequence":"additional","affiliation":[{"name":"Tianjin University , , ,","place":["Tianjin, China, 300072"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-0772-6782","authenticated-orcid":true,"given":"Zhao","family":"Wang","sequence":"additional","affiliation":[{"name":"Tianjin University , , ,","place":["Tianjin, China, 300072"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,7,30]]},"reference":[{"issue":"6737","key":"2026081200064909700_cit1","doi-asserted-by":"publisher","DOI":"10.1126\/science.adn9388","article-title":"Hydrogenation of CO2 for sustainable fuel and chemical production","volume":"387","author":"Ye","year":"2025","journal-title":"Science"},{"key":"2026081200064909700_cit2","doi-asserted-by":"publisher","DOI":"10.1016\/j.cej.2025.161579","article-title":"Research progress and future prospects of chemical utilization of CO2","volume":"510","author":"Shi","year":"2025","journal-title":"Chem. 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