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The rapidly developing organic–inorganic hybrid chalcogenide solar cells have now become a hot topic of interest. However, the bandgap of inorganic ferroelectric materials with a typical chalcogenide structure is too wide to match the solar spectrum, while the ferroelectricity of organic-inorganic hybrid chalcogenide materials with a narrow bandgap, meth amide–lead–iodine, is not obvious, and the lead element causes environmental pollution. The recently discovered organic–inorganic hybrid material [C6N2H18]BiI5 with good ferroelectricity and the narrowest bandgap of molecular ferroelectrics can absorb visible light in the range of 380 nm to 660 nm, and compound [C6N2H18]SbI5 with the Bi cognate element Sb was also synthesized. In this paper, we designed the first experiment to prepare thin films by mixing and doping the above two materials in five different molar ratios, and we comparatively studied the changes in crystal structure, surface morphology, and photophysical properties of the prepared multicomponent hybrid films according to the mixing ratio. A theoretical model was developed to calculate and analyze the bandgap of the hybrid doped compounds and compare it with the experimental values. It was found that the absorption spectra of the multicomponent hybrid films were red-shifted relative to the original material, indicating that the forbidden bandwidth was reduced to absorb a wider range of visible light, and the reason for this was thought to be the narrowing of the bandgap due to doping. When the mixing ratio was 0.4:0.6, the bandgap was the narrowest and the light absorption was the best; the highest quality of the film was obtained when the mixing ratio was 0.5:0.5.