All-inorganic cesium lead bromide (CsPbBr3) perovskite is attracting growing interest as functional ma-terials in photovoltaics and other optoelectronic devices due to its superb stability. However, the fabri-cation of high-quality CsPbBr3 films still remains a big challenge by solution-process because of the low solubility of the cesium precursor in common solvents. Herein, we report a facile solution-processed ap-proach to prepare high-quality CsPbBr3 perovskite films via a two-step spin-coating method, in which the CsBr methanol/H2O mixed solvent solution is spin-coated onto the lead bromide films, followed by an isopropanol-assisted post-treatment to regulate the crystallization process and to control the film mor-phology. In this fashion, dense and uniform CsPbBr3 films are obtained consisting of large crystalline do-mains with sizes up to microns and low defect density. The effectiveness of the resulting CsPbBr3 films is further examined in perovskite solar cells (PSCs) with a simplified planar architecture of fluorine–doped tin oxide/compact TiO2/CsPbBr3/carbon, which deliver a maximum power conversion efficiency of 8.11%together with excellent thermal and humidity stability. The present work offers a simple and effective strategy in fabrication of high-quality CsPbBr3 films for efficient and stable PSCs as well as other opto-electronic devices.