organic components with inorganic cations such as cesium (Cs + ) and rubidium (Rb + ) ions can effectively improve the thermal stability. Recently, all-inorganic cesium lead halide perovskites (CsPbX 3 , X = I, Br, Cl, or mixed halides), which have higher melting points (in excess of 460 °C), [10] have been investigated as thermal stable photoabsorption materials. The CsPbI 2 Br perovskites, which possess a reasonable bandgap of 1.9 eV and considerable phase stability, were emphasized as the main research subject in previous work. [24][25][26][27][28][29][30] To improve the performance of CsPbX 3 -based PSCs, a series of work on composition [18,19] and fabrication [20][21][22][23][24] engineerings have been intensely carried out. Unfortunately, the CsPbX 3 perovskites generally require high-temperature annealing (>250 °C) to form black photovoltaic-active cubic phase, [27][28][29][30] which is energy-consuming and undesirable for multijunction tandem and flexible solar cells. Up to now, it is still challenging to obtain uniform and void-free CsPbX 3 perovskite films via low-temperature solution-processed methods, let alone room temperature (RT) based technologies.In this work, we demonstrate that coordinated solvent dimethylsulphoxide (DMSO) can effectively induce the RT formation of photovoltaic-active CsPbX 3 perovskites, and a simple RT solvent (DMSO) annealing (RTSA) treatment can controllably remove the high boiling point DMSO and result in highly uniform and void-free CsPbX 3 perovskite films, as well as a postannealing treatment at the moderate temperature of 120 °C can further improve the perovskite grain size and crystallinity. These results provide an approach to prepare high quality allinorganic CsPbX 3 perovskite films at RT or a relatively low temperature (<120 °C). Consequently, efficient inverted CsPbI 2 Brbased PSCs were achieved on both glass and flexible substrates.As previously reported, [27] the CsPbI 2 Br perovskite precursor solution in N,N-dimethylformamide (DMF) suffers from a low concentration (≈0.43 m) due to the solubility limitation of bromide. While for the perovskite precursor solution with DMSO as solvent, the stronger coordination interaction between DMSO and the perovskite precursor enables the concentration exceeding 2 m ( Figure S1, Supporting Information), resulting in thicker perovskite films with sufficient light absorption ( Figure S2, Supporting Information). Furthermore, All-inorganic cesium lead halide (CsPbX 3 ) perovskites have emerged as promising photovoltaic materials owing to their superior thermal stability compared to traditional organic-inorganic hybrid counterparts. However, the CsPbX 3 perovskites generally need to be prepared at high-temperature, which restricts their application in multilayer or flexible solar cells. Herein, the formation of CsPbX 3 perovskites at room-temperature (RT) induced by dimethylsulphoxide (DMSO) coordination is reported. It is further found that a RT solvent (DMSO) annealing (RTSA) treatment is valid to control the perovskite cryst...