AbstractSmart materials with circularly polarized luminescence (CPL) tunable ability show great potential for advanced information storage and encryption. While an effective integration of high photoluminescence quantum yield (PLQY) and facile regulation of CPL property in thin films are of great significance, it is challenging due to the scarcity of suitable materials and complexity of systems. Herein, a novel acid‐responsive CPL tunable molecule is designed by combining an aggregation‐induced emission (AIE) component (TPE), an acid‐responsive luminophore (Rhodol), and a chiral aniline. Benefitting by the “AIE” effect of TPE and acid‐sensitive nature of Rhodol, the acidified molecule (S‐Rhodol‐TPE) exhibits a high PLQY even when doped in the polymer substrate at high concentrations. In addition, due to the fluorescence resonance energy transfer (FRET) process between TPE and Rhodol, the emission color of S‐Rhodol‐TPE can be easily regulated by the doped ratio and acidified degree of S‐Rhodol‐TPE in the polymer film. This work exhibits a unique approach to achieving smart CPL‐tunable films with high PLQYs and multiple emission color‐regulation properties, which can undoubtedly facilitate the progress of CPL tunable materials.