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Rational design of assemblies requires understanding how their electronic structures can be tuned by various factors, such as precursor design and substrate choice. While phase transformations can significantly alter both structural and electronic properties, most reported cases involve changes in chemical composition or bonding configurations. In contrast, systematic studies of geometric relaxation, which is modulated without altering chemical identity, remain limited, as such transformations often demand high temperatures that risk side reactions. In this study, we demonstrate a room\u2010temperature phase transformation in a supramolecular self\u2010assembly of Ag\u2013carboxylate complexes derived from 3,5\u2010dinitrobenzoic acid on Ag(111), proceeding without any changes in chemical composition. Combining scanning tunneling microscopy and spectroscopy with density functional theory calculations, we track a stepwise transformation among three distinct hexagonal lattices. The transformation induces subtle geometric relaxation that strengthens metal\u2013molecule interactions, thereby modulating the collective electronic structure. Unlike previous studies on polymorphic organic assemblies, this work reveals a composition\u2010preserving, phase\u2010transformation\u2010driven route to modulate electronic structures in metal\u2013organic coordination assemblies, enabling tuning of physicochemical functionalities in surface\u2010confined molecular architectures.<\/jats:p>","DOI":"10.1002\/smll.202513441","type":"journal-article","created":{"date-parts":[[2026,2,6]],"date-time":"2026-02-06T12:04:32Z","timestamp":1770379472000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Electronic Structure Modulation via Composition\u2010Preserving Phase Transformations in Metal\u2013Organic Assemblies on the Surface"],"prefix":"10.1002","volume":"22","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-9078-2100","authenticated-orcid":false,"given":"Hyungjun","family":"Park","sequence":"first","affiliation":[{"name":"Department of Applied Chemistry School of 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