The direct synthesis of a chiral nematic liquid crystalline phase of AgNR@SiO2@cysteine@CsPbBr3 hybrid nanorods (HNRs) is reported. The circular dichroism spectra can be divided into three components: (1) the interband absorption–enhanced optical activity of structural arrangement of cysteine (cys) molecules, 200–320 nm, (2) the chiral nematic liquid crystalline arrangement of the Ag nanorods (AgNRs), 350–450 nm, and (3) the exciton adsorption edge of the perovskite, 500–550 nm. The polarizing optical microscope images indicate that the chiroptical response of perovskite arises from chiral nematic crystalline arrangement rather than cys‐induced electronic coupling between a chiral ligand and otherwise achiral perovskite quantum dots (QDs). The luminescent intensity of CsPbBr3 QDs in AgNR@SiO2@cys@CsPbBr3 HNRs is boosted 87‐fold due to the local surface plasmon resonance field enhancement effect. Furthermore, the high‐performance green light emitting diode is constructed employing AgNR@SiO2@cys@CsPbBr3 complexes, which exhibit excellent luminescent properties. This work contributes insights into structure–property relationships and this strategy promisingly provides guidance for the other inorganic chiral semiconductor suprastructures.