Chiral perovskites, which are applied to spin organic light-emitting diodes as a spin-induced spin selectivity (CISS) layer, have attracted increasing amounts of attention. A device based on a thicker perovskite CISS layer leads to strongly spin-polarized EL emission. However, chiral perovskite films suffer from poor device performance due to difficulties in carrier injection and film quality. The effects of antisolvent dripping on the chiroptical properties of chiral perovskite films were investigated. The rapid crystallization of chlorobenzene (CB)-treated films generated a high-quality film with fewer halide vacancies and a much greater strength of asymmetric hydrogen bonding. Accordingly, the inorganic structural distortion is greater, resulting in greater chiroptical activity. The chiral perovskite thickness affects the circularly polarized electroluminescence (CP-EL) of spin-OLEDs. The statistics relating device performance and thickness are presented. The spin current polarization degree of chiral perovskites reaches approximately 86%. The maximum CP-EL asymmetry factor (