As a candidate for next‐generation solar devices, perovskite solar cells are increasingly being studied for their rapid increased power conversion efficiency (PCE). One of the possible routes to further increase PCE is the introduction of polarization in the absorption layer which functions as a method for increasing the built‐in potential and reducing the interface barrier, leading to much improved carrier separation and extraction. This technique uses the principle of the piezophototronic effect utilized for obtaining enhanced optoelectronic performances. Herein, to introduce internal polarization while maintaining optical absorption performance of the perovskite, organic–inorganic hybrid perovskite composite film solar cells are fabricated by doping polarized polyvinylidenefluoride‐co‐trifluoroethylene (P(VDF‐TrFE)) into the perovskite. The composite film is polarized with an external potential, subsequently inducing the piezophototronic effect to enhance the performances of perovskite solar cells. Experimental results show that this simple polarization method has effectively improved several key characteristics of the solar cell. The PCE has reached up to 22.1%, the short‐circuit current (Jsc) increases to 24.2 mA cm−2, and the open‐circuit voltage (Voc) increases to 1.18 V.
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