2D Dion-Jacobson (DJ) chiral perovskite materials exhibit significant promise for developing high-performance circularly polarized light (CPL) photodetectors. However, the inherently thick nature of DJ-phase 2D perovskite single crystal limits their ability to differentiate CPL photons with the two opposite polarization states. In addition, the growth of DJ-phase perovskite single crystal thin films (SCTFs) has proven challenging due to the strong interlayer electronic coupling. Here, a nucleation-controlled strategy is employed to grow a novel DJ-phase perovskite [(R/S)-3APr]PbI