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Ternary organic solar cells, a single active layer comprising three different components, are demonstrated to be one of the most efficient ways to approach high‐performance organic solar cells. But nevertheless, most of the ternary organic solar cells are characterized by steady‐state measurements, which are helpful but inadequate to fully understand the underlying charge carrier behavior at a short time scale. Herein, a comparison of the steady‐state and time‐dependent measurements is used to investigate the functionality of non‐fullerene electron acceptors in ternary organic solar cells. The steady‐state measurements indicate that non‐fullerene electron acceptors enlarge the absorption range of the photoactive layer, suppress charge carrier recombination, reduce charge carrier transfer resistance, and thereby increase photocurrent in ternary organic solar cells. The time‐dependent measurements demonstrate that a short charge carrier extraction time and a high charge carrier mobility are responsible for enhanced photocurrent in ternary organic solar cells. A comprehensive method understanding the underlying of enhanced efficiency of ternary organic solar cells is provided herein. 

Abstract Flexible perovskite solar cells (f‐PSCs) have attracted great attention due to their promising commercial prospects. However, the performance off‐PSCs is generally worse than that of their rigid counterparts. Herein, it is found that the unsatisfactory performance of planar heterojunction (PHJ)f‐PSCs can be attributed to the undesirable morphology of electron transport layer (ETL), which results from the rough surface of the flexible substrate. Precise control over the thickness and morphology of ETL tin dioxide (SnO₂) not only reduces the reflectance of the indium tin oxide (ITO) on polyethylene 2,6‐naphthalate (PEN) substrate and enhances photon collection, but also decreases the trap‐state densities of perovskite films and the charge transfer resistance, leading to a great enhancement of device performance. Consequently, thef‐PSCs, with a structure of PEN/ITO/SnO₂/perovskite/Spiro‐OMeTAD/Ag, exhibit a power conversion efficiency (PCE) up to 19.51% and a steady output of 19.01%. Furthermore, thef‐PSCs show a robust bending resistance and maintain about 95% of initial PCE after 6000 bending cycles at a bending radius of 8 mm, and they present an outstanding long‐term stability and retain about 90% of the initial performance after >1000 h storage in air (10% relative humidity) without encapsulation.