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Here, we present an atmospheric-pressure spatial atomic layer approach that enables the single-step, open-air synthesis of zinc\u2013tin\u2013oxide (ZTO) thin films with lateral compositional gradients over 3-in. wafer-scale substrates. A custom reactor head with spatially tailored precursor delivery generates continuous and reproducible composition gradients in under 1 h without vacuum processing or sequential depositions. Comprehensive structural, morphological, optical, and compositional characterization confirms smooth lateral variations in ZTO film composition and crystallinity, with Sn\/Zn atomic ratios spanning approximately 0.4\u20130.8 across one of the films, forming unique material libraries in a single open-air deposition step. As a proof of concept, the graded ZTO films are integrated into chemiresistive sensor arrays comprising 20 compositionally distinct sensing columns on a single wafer, exhibiting composition- and temperature-dependent (at 200 \u00b0C) responses to volatile organic compounds within a single device platform. Additionally, electrical measurements performed across the gradient show unique current\u2013voltage properties at each composition, alluding to multi-usage in electronic applications within the same chip. This work establishes a scalable and cost-effective strategy for rapid fabrication of oxide material libraries and wafer-scale collective device assemblies under ambient conditions.<\/jats:p>","DOI":"10.1021\/acsami.6c12174","type":"journal-article","created":{"date-parts":[[2026,8,31]],"date-time":"2026-08-31T20:17:12Z","timestamp":1788207432000},"page":"48449-48463","source":"Crossref","is-referenced-by-count":0,"title":["Scalable Single-Step Open-Air Combinatorial Growth of Multifunctional Metal Oxide Thin Films by Spatial Atomic Layer Deposition"],"prefix":"10.1021","volume":"18","author":[{"ORCID":"https:\/\/orcid.org\/0000-0003-0415-7278","authenticated-orcid":true,"given":"Ahmed","family":"Shahin","sequence":"first","affiliation":[{"name":"University of Waterloo , , 200 University Ave. West , ,","place":["Waterloo, Canada, N2L 3G1"]},{"name":"University of Waterloo , , 200 University Ave. West , ,","place":["Waterloo, Canada, N2L 3G1"]},{"name":"Institute for Quantum Computing, University of Waterloo , 200 University Ave. West , ,","place":["Waterloo, Canada, N2L 3G1"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0005-7271-690X","authenticated-orcid":true,"given":"Agosh","family":"Saini","sequence":"additional","affiliation":[{"name":"University of Waterloo , , 200 University Ave. West , ,","place":["Waterloo, Canada, N2L 3G1"]},{"name":"University of Waterloo , , 200 University Ave. West , ,","place":["Waterloo, Canada, N2L 3G1"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0007-1200-1560","authenticated-orcid":true,"given":"Denys","family":"Vidish","sequence":"additional","affiliation":[{"name":"University of Waterloo , , 200 University Ave. West , ,","place":["Waterloo, Canada, N2L 3G1"]},{"name":"University of Waterloo , , 200 University Ave. West , ,","place":["Waterloo, Canada, N2L 3G1"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Mahdi Hasanzadeh","family":"Azar","sequence":"additional","affiliation":[{"name":"University of Waterloo , , 200 University Ave. West , ,","place":["Waterloo, Canada, N2L 3G1"]},{"name":"University of Waterloo , , 200 University Ave. West , ,","place":["Waterloo, Canada, N2L 3G1"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-0290-7728","authenticated-orcid":true,"given":"Na Young","family":"Kim","sequence":"additional","affiliation":[{"name":"University of Waterloo , , 200 University Ave. West , ,","place":["Waterloo, Canada, N2L 3G1"]},{"name":"Institute for Quantum Computing, University of Waterloo , 200 University Ave. West , ,","place":["Waterloo, Canada, N2L 3G1"]},{"name":"University of Waterloo , , 200 University Ave. West , ,","place":["Waterloo, Canada, N2L 3G1"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-9752-0015","authenticated-orcid":true,"given":"Kevin P.","family":"Musselman","sequence":"additional","affiliation":[{"name":"University of Waterloo , , 200 University Ave. West , ,","place":["Waterloo, Canada, N2L 3G1"]},{"name":"University of Waterloo , , 200 University Ave. West , ,","place":["Waterloo, Canada, N2L 3G1"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,8,24]]},"reference":[{"key":"2026092209082368500_cit1","doi-asserted-by":"publisher","first-page":"64","DOI":"10.1007\/S10904-025-03707-6\/TABLES\/2","article-title":"Transformative Applications of Polymer-Based Metal Oxide Nanocomposites in Medicine, Industry, and Environmental Remediation: A Review","volume":"36","author":"Losetty","year":"2025","journal-title":"J. Inorg. Organomet. Polym. Mater."},{"issue":"9","key":"2026092209082368500_cit2","doi-asserted-by":"publisher","first-page":"706","DOI":"10.1038\/S41578-020-0212-2","article-title":"Mechanical Properties and Deformation Mechanisms of Gradient Nanostructured Metals and Alloys","volume":"5","author":"Li","year":"2020","journal-title":"Nat. Rev. Mater."},{"issue":"3","key":"2026092209082368500_cit3","doi-asserted-by":"publisher","first-page":"154","DOI":"10.1021\/ACSCOMBSCI.5B00146","article-title":"Geometry of Chemical Beam Vapor Deposition System for Efficient Combinatorial Investigations of Thin Oxide Films: Deposited Film Properties versus Precursor Flow Simulations","volume":"18","author":"Wagner","year":"2016","journal-title":"ACS Comb. 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