LAUSR

Chirality induction in aprotic polar solvents is challenging due to disrupted intermolecular interactions and the high conformational flexibility of random‐coil polymers. Herein, a scalable strategy using chiral BINOL as the sole chiral source to induce helical chirality in random‐coil polymers is presented. Circular dichroism (CD), ultraviolet‐visible (UV– vis), and resonance Raman spectroscopy confirm that chiral BINOL effectively induces cis‐transoidal helical conformations through hydrogen bonding and π–π stacking interactions. CD and circularly polarized luminescence (CPL) measurements reveal efficient chirality transfer and amplification, with mirror‐image CPL signals observed at 390 nm. Resonance Raman spectra demonstrate enhanced structural order and reduced irregularities, evidenced by a blue shift and narrowed C═C Raman peak, while achiral BINOL exhibits minimal induction ability. This study highlights the mechanisms of chirality induction and CPL excitation in random‐coil polymers in aprotic polar solvents, providing a versatile pathway for designing advanced materials with exceptional chiral optical and fluorescence properties.