In this work, doping 3-amino-propyl triethoxysilane (APTES) into a perovskite precursor is proven to be an effective strategy, which can passivate crystal defects, control the crystallization rate, and improve the morphology. APTES can form oligomers through hydrolysis and a condensation reaction, thus blocking the invasion of external water molecules. In addition, the lone pair electrons on the N atom in the amino group of APTES form a coordination bond with perovskite by sharing the empty 6p orbital on Pb 2+ , which can effectively passivate the defects of the film and realize a highly uniform and dense perovskite film with preferential crystal growth orientation. The film exhibits high (110) crystal plane orientation and long carrier lifetime and mobility, which improves the performance of flexible perovskite solar cells. Using this approach, the champion device presents an optimal power conversion efficiency of 19.84% with much promoted air stability. Moreover, the efficiency of flexible devices does not decrease after maximum power point irradiation for 360 s.