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Here, poly [bis(4\u2010phenyl)(2,4,6\u2010trimethylphenyl)amine] (PTAA) is employed as a model system to systematically explore how solvent\u2010PTAA interactions govern HTL wettability and the microstructure of metal halide perovskite (HP) films. Solvents with a dielectric constant (\n                    <jats:italic>\u03b5<\/jats:italic>\n                    <jats:sub>r<\/jats:sub>\n                    ) &gt; 15 are poor solvents, while their interactions with PTAA critically determine its wettability and the quality of HP films. Alcohols form weak\n                    <jats:italic>n<\/jats:italic>\n                    \u2192\n                    <jats:italic>\u03c0<\/jats:italic>\n                    <jats:sup>*<\/jats:sup>\n                    interactions with PTAA, yielding only marginal improvements. In contrast, the widely used N, N\u2010Dimethylformamide (DMF) induces strong\n                    <jats:italic>n<\/jats:italic>\n                    \u2192\n                    <jats:italic>\u03c0<\/jats:italic>\n                    <jats:sup>*<\/jats:sup>\n                    interactions that fracture the PTAA layer, leading to a defective interface. Remarkably, acetone provides an optimal interaction strength between carbonyl groups (C = O) of the solvent and the aromatic rings of PTAA, which enhances wettability while preserving HTL integrity by forming a polarity\u2010compatible interface with the HP precursor solution. This universal enhancement in quality of both three\u2010dimensional (3D) and low\u2010dimensional (LD) HPs boosts the power conversion efficiencies (PCEs) of corresponding solar cells (SCs) to 22.85% and 17.45% with increases of \u223c12% and \u223c25%, respectively, over DMF\u2010treated counterparts. This work offers a molecular\u2010level insight into solvent\u2010HTL interactions for advancing HPSCs.\n                  <\/jats:p>","DOI":"10.1002\/smll.76057","type":"journal-article","created":{"date-parts":[[2026,9,30]],"date-time":"2026-09-30T14:23:38Z","timestamp":1790778218000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Unveiling the Role of Solvent\u2010Hole Transport Layer Interactions in the Performance of Perovskite Solar Cells"],"prefix":"10.1002","author":[{"given":"Hui","family":"Zhang","sequence":"first","affiliation":[{"name":"Institute of Molecular Aggregation Science Tianjin University  Tianjin China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jianing","family":"Duan","sequence":"additional","affiliation":[{"name":"School of Electronic Science and Engineering Key Laboratory for Physical Electronics and Devices of the Ministry of Education &amp; Shaanxi Key Lab of 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