AbstractCPL‐active flexible materials with high luminescence dissymmetry factor (glum) and luminescent quantum yield are indispensable for 3D displays, wearable devices and so on. Perovskite has drawn much attention due to its fascinating photoelectric properties as well as its abundant applications. However, the existing strategies are inefficient in acquiring perovskite NCs with high glum. In this work, thermoregulated CPL‐active flexible polymer/perovskite hybrid materials with high glum by the creation of chiral photonic bandgap in polymer film with cholesteric domains using toluene as the dielectric media is reported. Based on selective CPL reflection, a satisfied CPL with a maximum glum of 0.6 is achieved. Importantly, the chiral photonic bandgap center of the polymer film can be easily tuned by thermal annealing at different temperatures to adapt various perovskite NCs with full‐spectral emission. The handedness of CPL of hybrid materials can be regulated with and without dielectric media. The presence of the flexible polymer makes hybrid materials a candidate to achieve patterned display applications. Additionally, the polymer/perovskite hybrid materials show excellent stability thanks to the encapsulation effect from polymers. This work provides a facile and general approach to induce adjustable CPL in the whole visible spectrum with high glum and photoluminescence quantum yield (PLQY).
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