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The organic-inorganic hybrid quasi-two-dimensional (quasi-2D) perovskites have attracted increasing attention for solar cell applications due to their improved moisture stability and excellent optoelectronic properties. To achieve a profound understanding and delicate control on the component of perovskite, it is indispensable to know how different spacer cations affect their intrinsic properties. Here, we synthesized a series of quasi-2D perovskite single crystals with different organic spacer cations and conducted a systematic invest