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Organometal halides are promising materials for photovoltaic applications, offering tunable electronic levels, excellent charge transport, and simplicity of thin-film device fabrication. Two-dimensional (2D) perovskites have emerged as promising candidates over three-dimensional (3D) ones due to their interesting optical and electrical properties. However, maximizing the power conversion efficiency is a critical issue to improve the performance of these solar cells. In this work, we studied the photophysics of a two-dimensional (2D) perovskite (CH3NH3)2Pb(SCN)2I2 thin film using steady-state and time-resolved absorption and emission spectroscopy and compared it with the three-dimensional (3D) counterpart CH3NH3PbI3. We observed a higher bandgap and faster charge recombination in (CH3NH3)2Pb(SCN)2I2 compared to CH3NH3PbI3. This work provides an improved understanding of fundamental photophysical processes in perovskite structures and provides the guideline for the design, synthesis, and fabrication of solar cells.