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The defects within perovskite films are the fatal roadblock limiting the performance of perovskite solar cells (PSCs). Herein, we develop a patching strategy to obtain high‐quality perovskite film using bifunctional trifluorophenylacetic acid (TFPA). Theoretical calculation and experiments reveal that the –COOH groups in TFPA effectively passivate the deep‐energy‐level defects of perovskite by combining with Pb clusters on the perovskite grain surfaces to enhance the efficiency of PSCs, and hydrophobic benzene groups containing fluorine in TFPA are exposed to improve the stability of PSCs. The power conversion efficiency (PCE) of PSCs with TFPA is enhanced from 22.95% to 24.56%. Most importantly, we successfully fabricated flexible PSCs using TFPA with the high PCE of 22.65%. The devices with TFPA maintain 93.22% of the initial efficiency MPP under continuous irradiation for 10.5 h, while the devices without TFPA only retain 82.22% of the initial efficiency under the same conditions for just 5 h. Meanwhile, the unsealed devices with TFPA hold 93.59% of the initial efficiency when stored in air for 3912 h. [ABSTRACT FROM AUTHOR]