As a type of ionic crystal, CsPbI2Br perovskite inevitably generates a significant number of defects during the rapid crystallization process that occurs from deposition to annealing. The non-radiative recombination of charge carriers caused by these defects severely limits the performance of perovskite solar cells (PSCs). Here, 2,2,2-trifluoroethylamine hydrochloride (F3EACl) with permanent dipole moment is devised to modify the perovskite interface. Highly electronegative trifluoro groups can accelerate the dielectric response of perovskite films, intensify the dielectric screening effect, and significantly suppress non-radiative recombination of charge carriers. Meanwhile, the –NH3+ group in F3EACl effectively passivates the defects at the perovskite surface, further alleviating the defect-induced carrier recombination loss. Consequently, the CsPbI2Br carbon-based PSCs treated with F3EACl achieved an impressive power conversion efficiency (PCE) of 14.69 % at a higher open-circuit voltage (1.28 V), along with excellent environmental stability. This work demonstrates a unique tactic to achieve efficient and stable PSCs by modulating charge carrier recombination utilizing the synergistic effects of dielectric screening and defect passivation.