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Here, we report a facile design strategy for FeMgAlOx solid\u2010solution catalysts featuring abundant active sites and enhanced interfacial structures that suppress nanocluster agglomeration. The successful synthesis of this catalyst relies on a high\u2010temperature\u2010induced two\u2010step strategy: high\u2010temperature oxidation enhances crystallinity, while high\u2010temperature air\/CO\n                    <jats:sub>2<\/jats:sub>\n                    treatment facilitates the formation of strong metal\u2010support interactions (SMSI) on inert metal oxide supports. In this architecture, the ultrathin two\u2010dimensional morphology and ordered atomic arrangement promote active\u2010metal spillover, yielding abundant active sites; meanwhile, CO\n                    <jats:sub>2<\/jats:sub>\n                    induction significantly enhances the SMSI\u2010mediated confinement capability for Fe nanoclusters. Crystalline evolution and SMSI regulation synergistically facilitate the exsolution of active Fe species from the bulk solid solution, thereby forming thermally stable Fe nanoclusters. Furthermore, optimized single\u2010walled carbon nanotube (SWCNT) growth kinetics confirm that the modified solid solution possesses both a higher density of active sites and enhanced intrinsic catalytic activity. Ultimately, our catalyst enables the growth of SWCNTs with diameters ranging from 0.96 to 3.33\u00a0nm, offering a simple and low\u2010cost route for SWCNT synthesis with broad application prospects.\n                  <\/jats:p>","DOI":"10.1002\/smll.76090","type":"journal-article","created":{"date-parts":[[2026,10,4]],"date-time":"2026-10-04T14:01:50Z","timestamp":1791122510000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Air\/CO\n                    <sub>2<\/sub>\n                    Stepwise Induction of Fe Nanocluster Enrichment in FeMgAlOx Solid\u2010Solution Catalysts for Single\u2010Walled Carbon Nanotube Growth"],"prefix":"10.1002","author":[{"given":"Peng","family":"Wang","sequence":"first","affiliation":[{"name":"Shandong Engineering Laboratory for Preparation and Application of High\u2010performance Carbon\u2010Materials, College of Electromechanical Engineering Qingdao University of Science and Technology  Qingdao China"},{"name":"ShangDong Dazhan Nano Materials Co., Ltd  Zouping China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Chenyu","family":"Gao","sequence":"additional","affiliation":[{"name":"Shandong Engineering Laboratory for Preparation and Application of High\u2010performance Carbon\u2010Materials, College of Electromechanical Engineering Qingdao University of Science and Technology  Qingdao China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-0266-1799","authenticated-orcid":false,"given":"Zhaoying","family":"Li","sequence":"additional","affiliation":[{"name":"College of Mechanical and Electrical Engineering Qingdao University  Qingdao China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0007-7765-2049","authenticated-orcid":false,"given":"Dianming","family":"Chu","sequence":"additional","affiliation":[{"name":"Shandong Engineering Laboratory for 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