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We design and synthesize bis\u2010sulfonimide\u2010functionalized fulleropyrrolidine derivatives grafted with nonionic sidechains. C60\u2010BSI\u2010PS, incorporating phosphonate ester sidechains, exhibits superior electronic properties compared to its carbonate\u2010ester counterpart and outperforms benchmark fulleropyrrolidine with ionic sidechains. These characteristics promote efficient charge\u2010transport and suppress recombination even under thick\u2010film conditions. The phosphonate ester groups also endow C60\u2010BSI\u2010PS with high solubility in ethanol, eliminating the need for toxic halogenated solvents or methanol. When processed from ethanol, the C60\u2010BSI\u2010PS interlayer delivers a power conversion efficiency (PCE) of 19.76% in PM6:D18:L8\u2010BO\u2010based OSCs, alongside excellent operational stability. It retains &gt;94% of its optimal PCE even at an ultra\u2010thick coating of 81\u00a0nm. The broad applicability of C60\u2010BSI\u2010PS is further demonstrated across leading binary, ternary, and quaternary OSC systems, achieving PCEs 21.11% for small\u2010area devices (0.04\u00a0cm\n                    <jats:sup>2<\/jats:sup>\n                    ) and 19.69% for large\u2010area devices (0.6\u00a0cm\n                    <jats:sup>2<\/jats:sup>\n                    ) in D18:L8\u2010BO:BTP\u2010eC9\u2010based system. Thus, engineering fullerene\u2010based materials through judicious sidechain functionalization is a powerful strategy for creating high\u2010performance, sustainable interlayers, paving the way for next\u2010generation photovoltaic technologies.\n                  <\/jats:p>","DOI":"10.1002\/anie.2886303","type":"journal-article","created":{"date-parts":[[2026,5,15]],"date-time":"2026-05-15T14:43:18Z","timestamp":1778856198000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":1,"title":["Revitalizing Fulleropyrrolidine via Nonionic Sidechain Engineering: An Ethanol\u2010Processible Interlayer Enabling Efficient Organic Solar Cells"],"prefix":"10.1002","volume":"65","author":[{"given":"Yanhui","family":"Fan","sequence":"first","affiliation":[{"name":"State Key Laboratory of Chemical Resource Engineering Beijing Advanced Innovation Center for Soft Matter Science and Engineering College of Chemistry Beijing University of Chemical 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