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Two-dimensional (2D) hybrid perovskite solar cells have induced widespread research interest owing to their higher stability as compared to three-dimensional (3D) analogues. The photovoltaic performance, however, is still limited. Here, we report a perovskite film dominated by 3D components that are modulated by formamidinium thiocyanate in the 2D PEA(2)FA(3)Pb(4)I(13) perovskite composition. We demonstrate that a dimensionality transformation from a 2D/3D to predominantly 3D perovskite phase in the presence of SCN-based treatment enhances the optical absorption in visible and near-infrared regions. As a result, the power conversion efficiency improved 4.5 times with respect to the control to above 14%. The unencapsulated cell exhibited excellent moisture stability during the shelf lifetime measurement over 70 days under ambient conditions.