The strong ionic character endows all‐inorganic CsPbX3 (X = Cl, Br, I) perovskite nanocrystals (NCs) with different chemical features from classical Cd‐based NCs, especially when considering their interaction with polar solvents and surfactants. This has aroused intensive interest, but is still short of comprehensive understanding. More significantly, above characteristic may be used to improve the quality of perovskite thin films, which is crucial for the carrier transport inside optoelectronic devices. Here, an interesting recyclable dissolution–recyrstallization phenomenon of all‐inorganic pervoskite, as well as its application on room temperature (RT) self‐healing of compact and smooth carrier channels in ambient atmosphere for high‐performance PDs with high stability is reported. First, according to solubility equilibrium principle, the size of CsPbBr3 crystals can be reversibly tuned in the range of 10 nm–1 μm through washing with polar solvent or stirring with assistance of surfactants at RT. Second, such phenomenon is applied for significant film quality improvement by forming a liquid circumstance within films, which can transport matter at surface and sharp parts into the gaps, healing themselves at RT. This strategy results in large‐area, crack‐free, low‐roughness perovskite thin films. Obviously, such improvement facilitates transport and extraction of carriers in the channels of devices, which has been evidenced by the improvement of performances of the corresponding PDs at ambient condition.