All-inorganic lead halide perovskites are promising materials for many optoelectronic applications. However, two issues that arise during device fabrication hinder their practical use, namely, inadequate continuity of coated inorganic perovskite films across large areas and inability to integrate these films with traditional photolithography due to poor adhesion to wafers. Herein, for the first time, to address these issues, we show a room-temperature synthesis process employed to produce CsPbBr₃ perovskite nanocrystals with two-dimensional (2D) nanosheet features. Due to the unique properties of these 2D nanocrystals, including the “self-assembly” characteristic, the “double solvent evaporation inducing self-patterning” strategy is used to generate high-quality patterned thin films in selected areas automatically after drop-casting, enabling fabrication of high-performance devices without using complex and …