Most solution‐based synthetic routes for perovskite film deposition take place under highly controlled atmospheres and cannot be easily escalated for mass production. Here, the control in situ over luminescent, morphological, and structural characteristics of hybrid and inorganic perovskite films deposited on top of hot glass substrates by multisource AACVD is reported. By simply adjusting the methylammonium chloride (MACl) to lead bromide (PbBr2) molar ratio in the N‐N dimethylformamide (DMF) precursor solution, a gradual transformation from orthorhombic PbBr2 to cubic MAPbBr2Cl hybrid perovskite films is observed, and the generation of highly luminescent MAPbBr3−xClx nanoparticulate domains in a PbBr2 matrix is easily achieved when a specific ratio is used. Additionally, the crystallization of the films is performed in situ modified by the implementation of an antisolvent stream source during deposition which in turn yields films with superior luminescence properties. Finally, an NIR emitting CsPbBr2Cl:Yb inorganic perovskite film is deposited to probe the versatility of the multisource AACVD system, by the simultaneous deposition of separated PbBr2/YbCl3·6H2O/DMF and CsCl/methanol solutions. The high degree of control on the final properties of the films indicates that AACVD could be a breakthrough for low‐cost, scalable, high‐throughput metal‐halide perovskite film deposition.
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