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To address this, we designed two fullerene\u2010based self\u2010assembled monolayers (SAMs)\u2014C2\u2010PA and 4EG\u2010PA\u2014as interfacial modifiers for zinc oxide (ZnO). Systematic comparisons reveal that the tetra(ethylene glycol) linker in 4EG\u2010PA induces a denser and more uniform SAM morphology than the alkyl chain in C2\u2010PA, which more effectively passivates the polar ZnO surface. This superior molecular packing translates into a champion power conversion efficiency of 19.46%. More critically, transient absorption spectroscopy (TAS) provides direct evidence that the 4EG\u2010PA\u2010modified interface facilitates the formation of a favorable charge\u2010transfer state, which not only promotes electron extraction but also enhances hole transfer efficiency from the acceptor to the donor, thereby suppressing non\u2010geminate recombination. Concurrently, the dense SAM acts as a robust buffer, improving the thermodynamic compatibility with the active layer and inhibiting its deleterious reaggregation. This dual mechanism\u2014enhanced charge extraction and optimized interfacial morphology\u2014underpins the exceptional operational stability, with devices retaining 84% of their initial performance after 2000 h. Our work elucidates the critical link between SAM molecular structure, interfacial properties, and device longevity, providing a strategic blueprint for future interfacial material design.<\/jats:p>","DOI":"10.1002\/smll.202513104","type":"journal-article","created":{"date-parts":[[2026,1,30]],"date-time":"2026-01-30T14:59:11Z","timestamp":1769785151000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":3,"title":["Toward a Robust ZnO Interface via Fullerene\u2010Based SAMs: Defect Passivation and Compatibility Tuning for High\u2010Performance Inverted Organic Solar Cells"],"prefix":"10.1002","volume":"22","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-1917-5674","authenticated-orcid":false,"given":"Tian","family":"Xia","sequence":"first","affiliation":[{"name":"Department of Materials Science and Engineering City University of Hong Kong  Kowloon Hong Kong P. R. 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