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Here, we design geometrically asymmetric zwitterions, featuring a bulky charge\u2010dispersed triphenylphosphonium cation and a small charge\u2010concentrated sulfonate anion linked by an alkyl chain, to weaken intermolecular and intramolecular charge attraction, thereby constructing a permanent dipole interlayer that mitigates such recombination. By extending the alkyl spacer and introducing methyl substituents on triphenylphosphonium, the optimized zwitterion, 4\u2010(tri\u2010p\u2010tolylphosphonio)butane\u20101\u2010sulfonate (4MePS), achieves an ultrahigh dipole moment of 14.92\u00a0Debye. 4MePS strongly interacts with both perovskite and TiO\n                    <jats:sub>2<\/jats:sub>\n                    to form surface dipoles, drastically lowering their work functions by 0.42 and 0.54\u00a0eV, respectively. Comprehensive characterizations confirm that 4MePS suppresses non\u2010radiative recombination and accelerates charge extraction in p\u2010MPSCs. Consequently, 4MePS\u2010treated p\u2010MPSCs deliver a champion power conversion efficiency (PCE) of 23.3% (vs. 21.8% for control) and a minimodule efficiency of 20.2% over 57.3\u00a0cm\n                    <jats:sup>2<\/jats:sup>\n                    , among the highest reported for p\u2010MPSCs. Encapsulated devices retain 90% of their initial PCE after 1200\u00a0hours of maximum power point tracking under 1\u2011sun illumination at 55\u00a0\u00b1\u00a05\u00a0\u00b0C. This work establishes a charge density\u2010asymmetric molecular design strategy for engineering interfacial dipoles toward high\u2010performance perovskite devices.\n                  <\/jats:p>","DOI":"10.1002\/adma.74629","type":"journal-article","created":{"date-parts":[[2026,8,19]],"date-time":"2026-08-19T10:41:54Z","timestamp":1787136114000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Geometrically Asymmetric Phosphonium Zwitterions Enable Efficient Printable Mesoscopic Perovskite Solar Cells"],"prefix":"10.1002","volume":"38","author":[{"given":"Jianhang","family":"Qi","sequence":"first","affiliation":[{"name":"Michael Gr\u00e4tzel Center for Mesoscopic Solar Cells Wuhan National Laboratory for Optoelectronics Key Laboratory of Materials Chemistry for Energy Conversion and Storage of Ministry of Education Huazhong University of Science and Technology Wuhan Hubei 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National Laboratory for Optoelectronics Key Laboratory of Materials Chemistry for Energy Conversion and Storage of Ministry of Education Huazhong University of Science and Technology Wuhan Hubei China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Kai","family":"Chen","sequence":"additional","affiliation":[{"name":"Michael Gr\u00e4tzel Center for Mesoscopic Solar Cells Wuhan National Laboratory for Optoelectronics Key Laboratory of Materials Chemistry for Energy Conversion and Storage of Ministry of Education Huazhong University of Science and Technology Wuhan Hubei China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0006-7271-0767","authenticated-orcid":false,"given":"Yang","family":"Zhou","sequence":"additional","affiliation":[{"name":"Michael Gr\u00e4tzel Center for Mesoscopic Solar Cells Wuhan National Laboratory for Optoelectronics Key Laboratory of Materials Chemistry for Energy Conversion and Storage of Ministry of 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