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A star hybrid inorganic–organic perovskite material selected as an outstanding absorbing layer in solar cells benefits from multiple preparation techniques and excellent photoelectric characteristics. Among numerous synthetic processes, uniform, compact, and multi-stack perovskite thin films can be manufactured using vacuum deposition. During sequential vacuum deposition, the penetration ability of the organic molecules cannot be effectively controlled. In addition, the rela-tionship between the thickness of the inorganic seeding layer and the organic molecule concentration for optimized devices using an evaporation–solution method is unclear. In this work, we prepared high-quality perovskite films by effectively con-trolling the penetration ability and chemical quantity of organic methyl ammonium iodide by monitoring the evaporation pressure and time. Thus, a device efficiency of over 15％was achieved with an all-vacuum prepared perovskite film. For the evaporation–solution method, we reacted different thicknesses of inorganic lead iodine with various concentrations of the organic molecule solution. The inorganic layer thickness and organic molecule concentration showed a linear relationship to achieve an optimum perovskite film, and an empirical formula was obtained. This work noted the key parameters of two intercalation reactions to prepare perovskite films, which paves a way to deliver a device that enables multi-layered structures, such as tandem solar cells.