The in situ deposition of emerging organic–inorganic metal halides (OIMHs) films on glass or stretchable substrates has been challenging, and no methodology has been reported to achieve this goal. The aerosol‐assisted chemical vapor deposition technique using an antisolvent‐enhanced crystallization process (AEC–AACVD) is a simple, cost‐effective, scalable, and high‐throughput technique operated under ambient atmosphere and pressure. The AEC–AACVD technique (an all‐green chemistry methodology) is used in this work to deposit TPA2MnCl2Br2 luminescent films on glass and highly stretchable elastomer substrates. The effect of using different antisolvents on the structural, morphological, and photoluminescent (PL) characteristics of films deposited on glass is reported. It is found that the intensity of the characteristic green emission peaks at 511 nm for this OIMH, improving with the antisolvent application. The TPA2MnCl2Br2 films deposited using a mixture of antisolvents result in the maximum emission intensity when deposited on stretchable substrates, maintaining their overall PL characteristics. The processability, scalability, and performance reported here for these films prove their potential application in the next generation of OIMH‐based optoelectronic technologies.