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Here we report an efficient and reproducible multifunctional additive engineering strategy via methoxysilane cross-linking agents functionalized by the different terminal group, moderate electron-donating −SH, weak electron-donating −CH3, or strong electron-withdrawing −CN, into a PbI2 precursor solution. The power conversion efficiency (PCE) is increased from 18.4 to 20.8% after introduction of (3-mercaptopropyl)­trimethoxysilane (MPTS) containing a −SH group as a consequence of improved voltage and current density, while 3-cyanopropyltri­ethoxysilane (CPTS) containing a −CN group deteriorates the overall photovoltaic performance. Moreover, −SH in MPTS is found to passivate defects effectively through a Lewis acid–base interaction with PbI2, resulting in a larger grain size and a longer carrier lifetime. Owing to the formation of a cross-linking siloxane network as a protective layer on the grain boundary, the thermal and moisture stability of the device are improved remarkably. The present work provides a guideline for multifunctional additive engineering for the purpose of simultaneous achievement of a high PCE and long-term stability.

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