Multilayered chiral hybrid perovskites are highly desired for highly‐sensitive circularly polarized light (CPL) detection rooted in their efficient charge transport and strong chiroptical activity. However, designing multilayered chiral hybrid perovskites remains a huge challenge. Here, through pairing achiral ethylamine (EA)−chiral arylamine in the interlayer space, multilayered chiral alternating cations intercalation‐type (ACI) hybrid perovskites (R‐/S‐PPA) EA2Pb2Br7 (PPA = 1‐phenylpropylamine) are successfully obtained. Significantly, perovskitizer EA extends the thickness of the quantum well and alternating space cation EA greatly alleviates in‐plane tilting distortions of adjacent metal halide octahedra, providing fast channels for in‐plane carrier transport. Consequently, single‐crystal photodetectors of (R‐/S‐PPA) EA2Pb2Br7 exhibit high circular polarization sensitivity with a large anisotropy factor of 0.3, which falls around the highest value among the layered hybrid perovskites. In addition, a fast responding rate (τr )of 308 µs and a high CPL‐detectivity of 8 × 1012 Jones are also presented. This work opens up a new perspective to design multilayered chiral hybrid perovskites for high‐sensitive CPL detection. High‐sensitive circularly polarized light detection was realized in multilayered hybrid perovskite enantiomers which are designed by paring ethylamine and chiral arylamine cations in the interlayered space.