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Here, we propose a synergistic passivation strategy with 1\u2010dodecanethiol (DT) and 2\u2010mercaptobenzimidazole (MBI) into a low\u2010defect, ultrathin passivation film on copper. The molecularly engineered passivation film affords a four\u2010order\u2010of\u2010magnitude improvement in corrosion current suppression. Notably, the Cu\u2010DT\u2010MBI preserves this four\u2010order\u2010of\u2010magnitude protection even after 24\u2010h immersion in 1\u00a0M NaOH and maintains effective corrosion resistance for more than 13 days. A combination of in situ spectroscopy and cross\u2010sectional electron microscopy reveals a uniform and continuous passivation film with a thickness of 1.03\u00a0nm. The enhanced protection is attributed to the functional complementarity between DT and MBI: DT contributes a hydrophobic alkyl\u2010chain barrier, while MBI preferentially coordinates with under\u2010coordinated Cu sites and improves interfacial continuity. DFT calculations further indicate that the passivated surface weakens O\n                    <jats:sub>2<\/jats:sub>\n                    and Cl\n                    <jats:sup>\u2212<\/jats:sup>\n                    adsorption, thereby suppressing oxidation and corrosion. Furthermore, a roll\u2010to\u2010roll manufacturing process was demonstrated to produce passivated Cu foils that retain excellent conductivity while withstanding harsh alkaline attack. This work provides a foundational framework for designing ultra\u2010stable molecular interfaces via synergistic passivation.\n                  <\/jats:p>","DOI":"10.1002\/smll.74440","type":"journal-article","created":{"date-parts":[[2026,7,6]],"date-time":"2026-07-06T05:52:29Z","timestamp":1783317149000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Defect\u2010Suppressed Molecular Passivation Film Endure the Trade\u2010Off: Scalable Co\u2010Passivation for Copper That Withstands Harsh Alkaline Attack"],"prefix":"10.1002","volume":"22","author":[{"given":"Zhen","family":"Xu","sequence":"first","affiliation":[{"name":"State Key Laboratory of Advanced Technology For Materials Synthesis and Processing Wuhan University of Technology  Wuhan China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yanjuan","family":"Long","sequence":"additional","affiliation":[{"name":"School of Environment and Energy South China University of Technology  Guangzhou China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Dongxue","family":"Wang","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Advanced Technology For Materials Synthesis and Processing Wuhan University of Technology  Wuhan China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xiaomeng","family":"She","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Advanced Technology For Materials Synthesis and Processing Wuhan University of Technology  Wuhan China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Chi","family":"Zhang","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Advanced Technology For Materials Synthesis and Processing Wuhan University of Technology  Wuhan China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Junhao","family":"Zhou","sequence":"additional","affiliation":[{"name":"State Key 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