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HighlightsOxyacid anions (NO 3  − , SO 4  2− , CO 3  2− , PO 4  3−  and SiO 3  2− ) were investigated both theoretically and experimentally about their passivation effect on CsPbI 2 Br perovskite interface.    Adjustment of oxysalt layer thickness can optimize the surface band position that could be beneficial for electronic band alignment at perovskite/transport layer interface.    Using silicate as a passivator, the CsPbI 2 Br solar cells achieved a PCE of 17.26% with an open-circuit voltage of 1.36 V. This strategy is also effective for organic-inorganic perovskite solar cells.Electronic supplementary material  The online version of this article (10.1007/s40820-021-00683-7) contains supplementary material, which is available to authorized users.

Mediating the Local Oxygen-Bridge Interactions of Oxysalt/Perovskite Interface for Defect Passivation of Perovskite Photovoltaics