emergence of the hybrid organometal halide perovskite as photovoltaic absorbers had led to a breakthrough in the field of solar technologies. The perovskite-based solar cells (PSCs) had accomplished a dramatic enhancement in the power conversion efficiency (PCE) from 3.8% in 2009 [1] to a lately announced certificated PCE of 23.3%, [2] outperforming not only other emerging technologies, but also a number of well-established photovoltaic technologies. The superior properties of hybrid organometal halide perovskite materials include high absorption coefficients, tunable bandgaps, long carrier diffusion length, high carrier mobility, and low exciton binding energy making the material highly suitable for photovoltaic applications. [3][4][5][6] The theoretical maximum PCE for the CH 3 NH 3 PbI 3−x Cl x -based PSCs is found to be 31.4%, [7] which approaches the Shockley-Queisser limit of 33% achieved by gallium arsenide solar cells. [8] Tremendous research efforts had been devoted for optimizing the device architecture, as well as deposition techniques and composition of different layers, in particular the perovskite absorber. [9][10][11][12][13][14][15] It is well known that high efficiency and good stability PSCs require certain desirable perovskite film properties such as low defect density, high crystallinity, good coverage, and uniformity. [16][17][18][19] The perovskite films can be prepared by different methods, such as solution techniques, [20,21] thermal evaporation, [22][23][24] and a combination of vapor and the solution A cryogenic process is introduced to control the crystallization of perovskite layers, eliminating the need for the use of environmentally harmful antisolvents. This process enables decoupling of the nucleation and the crystallization phases by inhibiting chemical reactions in as-cast precursor films rapidly cooled down by immersion in liquid nitrogen. The cooling is followed by blow-drying with nitrogen gas, which induces uniform precipitation of precursors due to the supersaturation of precursors in the residual solvents at very low temperature, while at the same time enhancing the evaporation of the residual solvents and preventing the ordered precursors/perovskite from redissolving into the residual solvents. Using the proposed techniques, the crystallization process can be initiated after the formation of a uniform precursor seed layer. The process is generally applicable to improve the performance of solar cells using perovskite films with different compositions, as demonstrated on three different types of mixed halide perovskites. A champion power conversion efficiency (PCE) of 21.4% with open-circuit voltage (V OC ) = 1.14 V, short-circuit current density ( J SC ) = 23.5 mA cm −2 , and fill factor (FF) = 0.80 is achieved using the proposed cryogenic process.When humanity in the modern world consumes ever-increasing energy for the development of the infrastructure, growth of the economy and to raise the standard of living, securing clean and sustainable energy resources becomes a cri...