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The perovskite solar cells (PSCs) are promising for commercialization and practical application. However, high‐quality perovskite films are normally fabricated in inert gas‐filled glovebox, followed by thermal annealing, which is energy‐consuming and thus not cost‐effective. In this study, a simple manufacturing strategy is demonstrated to fabricate the highly‐crystalline perovskite films in ambient air (a relative humidity of over ≈50%) at room temperature via blade‐coating without the subsequent thermal–annealing. The perovskite precursor chemistry is tailored by solvent engineering via employing 2‐methoxyethanol, which can strongly coordinate with ammonium halide species, thus forming highly uniform small‐sized colloids and facilitating the homogeneous nucleation and rapid crystallization of perovskite films even at room temperature. The resultant PSCs fabricated with ambient‐processed, annealing‐free MAPbI3 perovskite films exhibit a champion efficiency up to 19.16% with negligible hysteresis and improved reproducibility, which is on par with the high‐temperature annealed counterparts fabricated in N2, and represented one of the highest reported efficiencies for the room‐temperature processed PSCs in ambient air. The unencapsulated devices show extended lifespan over 1000 h with nearly no efficiency loss. [ABSTRACT FROM AUTHOR]

Room temperature‐processed electron transport layers (RT‐ETLs) demonstrate vast potential to be used in fabricating high‐performance flexible perovskite solar cells (PSCs) in an energy‐saving manner. However, the RT‐ETL normally suffers from inferior crystallinity, mismatched energy level, and high surface trap‐state density, which would result in under‐optimized interfacial electron extraction and undesirable interfacial charge recombination at ETL/perovskite interface, thus limiting the device performance. Herein, a novel strategy is demonstrated to prepare annealing‐free RT‐ETL based on precrystalline metal ion‐modified SnO2 nanocrystals, which perfectly optimizes the interfacial energy level alignment between ETL and perovskite layer, achieving nearly zero‐barrier charge transfer at the interface. As a result, the charge extraction has been remarkably accelerated and the interfacial charge recombination has been largely suppressed, leading to a ≈26% enhancement in device efficiency. The best‐performing flexible PSCs achieve efficiencies up to 19.3%, accompanied by outstanding mechanical strength under repeated bending cycle tests, which, to the best of the knowledge, is one of the highest reported values for the flexible perovskite photovoltaics fabricated with RT‐ETLs. [ABSTRACT FROM AUTHOR]