Drying‐Mediated Spatial Confinement of Microcapsules Enables High‐Performance Multicolor Circularly Polarized Luminescence for Chiroptical Encryption and Display

Circularly polarized luminescent materials with high luminescence dissymmetry factor ( g lum ) are essential for practical photonic applications. However, achieving considerable chirality amplification through scalable solution‐processable methods remains highly challenging, due to the lack of long‐range chiral ordering in wet‐processed system. Here, we report a fully solution‐processable, drying‐driven microcapsule confinement strategy that transforms chiral liquid crystal microcapsules into high‐performance circularly polarized luminescence (CPL) films. Drying‐induced curvature modulation reorganizes the helical superstructure, yielding films with high dissymmetry factor ( g lum ) of 1.8. In‐situ characterization of individual microcapsule revealed that curvature variations boost the chiroptical signals. This approach is broadly compatible with diverse chromophores, enabling multicolor, white‐light, and upconverted CPL emission. Stochastic mixing of oppositely chiral CPL‐active inks further generates robust upconverted and downshifted physical unclonable functions with high randomness and stable readout. Moreover, multicolor CPL‐active inks allow facile patterning of chirality‐encoded images, enabling polarization‐selective and pseudo‐3D visualization. This versatile strategy provides a scalable platform for high‐performance CPL materials fabrication and chiroptical information encryption and display.