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Perovskite solar cells (PSCs) have attracted intense research interest due to their unique properties, including low cost, large-scale processability, and high efficiency. In the past several years, the PSC field has witnessed a remarkable increase in power conversion efficiency (PCE) from 3.8% to over 25%, [1] which was comparable to the most established decades-old commercial photovoltaic technologies. To date, most of the highly efficient PSCs were prepared by the solution-chemistry approach. [2][3][4][5][6][7] However, for scaled-up production, many issues, such as the wide processing window, light trapping (which has been widely used in traditional thinfilm solar cells), and fabrication of scaledup perovskite film with high-quality, remain to be solved.The "annealing window" (the storage time of the intermediate-state films As the power conversion efficiency (PCE) of perovskite solar cells (PSCs) is increased to as high over 25%, it becomes pre-eminent to study a scalable process with wide processing window to fabricate large-area uniform perovskite films with good light-trapping performance. A stable and uniform intermediate-state complex film is obtained by using tetramethylene sulfoxide (TMSO), which extends the annealing window to as long as 20 min, promotes the formation of a high-quality perovskite film with larger grains (over 400 nm) and spontaneously forms the surface texture to result in an improved fill factor and open-circuit voltage (V oc ). Moreover, the superior surface texture significantly increases the long-wavelength response, leading to an improved short-circuit current density (J sc ). As a result, the maximum PCE of 21.14% is achieved based on a simple planar cell structure without any interface passivation. Moreover, a large area module with active area of 6.75 cm 2 is assembled using the optimized TMSO process, showing efficiency as high as 16.57%. The study paves the way to the rational design of highly efficient PSCs for potential scaled-up production.

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