摘要： Advancements in exploring new chiral perovskites are highly demanded to improve the circular polarized light (CPL) detection efficiency to date. Reduced-dimensional (quasi-2D) perovskites thus emerged as the most promising candidates due to its appealing characteristics. We herein reported new chiral quasi-2D perovskite single crystals (SCs) synthesis, and investigate their CPL detecting capability for the first time. We proved quasi-2D chiral perovskites, [(R)-β-MPA]2MAPb2I7 ((R)-β-MPA = (R)-(+)-β-methylphenethylamine, MA = methylammonium), do possess intrinsic chirality and have the capability to distinguish different polarization states of CPL photons. Corresponding quasi-2D perovskite SCs CPL photodetector exhibit excellent detection performance. In particular, our device responsivity is almost one order of magnitude higher than the best reported 2D perovskite CPL detectors to date. On this basis, we carefully modulate the film’s crystallization dynamics to facilitate its carrier transport. We prove that parallelly oriented perovskite films with homogeneous energy landscape are crucial to maximize the device’s carrier collection efficiency. The obtained responsivity and linear dynamic range (LDR) of this flexible chiral quasi-2D perovskite thin-film photodetector are comparable with the best reported results to date. The photodetector also exhibits superior mechanical flexibility and durability, representing one of the most sensitive and robust CPL photodetector to date.