“…Chiral hybrid perovskites (CHPs), [ 9 , 10 ] featured with handedness sensitive absorption induced by chiral organic ligands and superior optoelectronic properties originating from inorganic frameworks, [ 11 , 12 , 13 , 14 , 15 , 16 , 17 ] are ideal candidates for the construction of high‐performance direct CPL detector. Over the past few years, thin‐film‐based CHPs photodetectors have enabled direct detection of light polarization states with enhanced responsivity; [ 18 , 19 , 20 , 21 , 22 ] however, the capability of these devices to distinguish CPL is still limited due to the introduction of impurities and intrinsic defect states during the rapid crystallization process. [ 23 ] With low defect density and long carrier diffusion length stemming from the long‐range crystallographic order, [ 24 , 25 , 26 , 27 , 28 ] high‐crystallinity CHP as active component affords an opportunity to detect CPL with high polarization discrimination ratio.…”