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In this work, we reveal the role of non-covalent interactions, which are known to play important roles in supramolecular phenomena, in achieving efficient perovskite surface and grain boundary passivation. By using a series of pseudohalides, we find that trifluoroacetate (TFA^-) provides the strongest binding to iodide vacancies by means of non-covalent hydrogen bonding and dispersion interactions. By exploiting additional non-covalent dispersion and hydrophobic interactions in aromatic 3,3-diphenylpropylammonium (DPA⁺), we present a dual-ion passivation strategy that not only minimizes the non-radiative recombination center and local chemical inhomogeneities but also induces preferentially oriented growth of α-FAPbI₃ lattice. Further, this leads to anmore » outstanding power conversion efficiency (PCE) of 25.63% with an exceptional open-circuit voltage of 1.191 V in a perovskite solar cell with a small area, while perovskite solar mini modules with aperture areas of 25 and 64cm² achieved PCE of 22.47% (quasi-steady-state [QSS]-certified 20.50%) and 20.88%, respectively, with outstanding stability under high-humidity conditions.« less