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Early studies focused mainly on the first coordination sphere; however, catalytic behavior is also shaped by second\u2010sphere interactions, support environments, extended spatial architectures, and their dynamic evolution. In this Review, we establish a cross\u2010scale framework for the rational design of SACs across interconnected design dimensions: from in\u2010plane to out\u2010of\u2010plane coordination; from primary coordination to through\u2010bond secondary\u2010sphere interactions, through\u2010space microenvironments and metal\u2013support interfaces; and from individual sites to macroscopic architectures governed by site density, intersite distance and topology. We further highlight directed dynamic reconstruction as an active design strategy that links as\u2010synthesized structures with catalytically relevant working states. By integrating static structure, working\u2010state evolution, and device operation, this Review provides insights into environment\u2010dependent performance and guides the rational design of SACs across scales.<\/jats:p>","DOI":"10.1002\/smll.75310","type":"journal-article","created":{"date-parts":[[2026,10,7]],"date-time":"2026-10-07T11:48:18Z","timestamp":1791373698000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Cross\u2010Scale Engineering of Single\u2010Atom Catalysts from Local Planar Coordination to Spatial Architectures"],"prefix":"10.1002","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-8019-0160","authenticated-orcid":false,"given":"Dazhi","family":"Yao","sequence":"first","affiliation":[{"name":"School of Chemistry University of New South Wales (UNSW Sydney)  Kensington New South Wales Australia"},{"name":"Tsinghua Center for Green Chemical Engineering Electrification Department of Chemical Engineering Tsinghua University  Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Siheng","family":"Yang","sequence":"additional","affiliation":[{"name":"Key Laboratory of Green Chemistry and Technology College of Chemistry Sichuan University  Chengdu Sichuan China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-6917-6800","authenticated-orcid":false,"given":"Shuhao","family":"Wang","sequence":"additional","affiliation":[{"name":"School of Chemistry University of New South Wales (UNSW Sydney)  Kensington New South Wales Australia"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-3027-0816","authenticated-orcid":false,"given":"Bernt","family":"Johannessen","sequence":"additional","affiliation":[{"name":"Australian Synchrotron Australian Nuclear Science and Technology Organization (ANSTO)  Clayton Victoria Australia"},{"name":"Institute for Superconducting and 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