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As one of the most frequently-used electron-transporting materials, the mesoporous titanium dioxide (m-TiO₂) film used in mesoporous structured perovskite solar cells (PSCs) can be employed for the scaffold of the perovskite film and as a pathway for electron transport, and the contact area between the perovskite and m-TiO₂ directly determines the comprehensive performance of the PSCs. Because of the substandard interface combining quality between the all-inorganic perovskite CsPbIBr₂ and m-TiO₂, the development of the mesoporous structured CsPbIBr₂ PSCs synthesized by the one-step method is severely limited. Here, we used a solution containing PbI₂, monoethanolamine (EA) and dimethyl sulfoxide (DMSO) (PED) as the interfacial modifier to enhance the contact area and modify the m-TiO₂/CsPbIBr₂ contact characteristics. Comparatively, the performance of the solar device based on the PED-modified m-TiO₂ layer has improved considerably, and its power conversion efficiency is up to 6.39%.