Mechanically‐Tunable and Full‐Color Circularly Polarized Long‐Lived Phosphorescence in Chiral Superstructure Elastomers

Abstract Developing full‐color circularly polarized organic ultralong room‐temperature phosphorescence (CP‐OURTP) materials with high dissymmetry factor ( g lum ) holds significant promise for diverse optoelectronic applications. Controlling g lum values is crucial for enhancing the performance and functionality of these materials, as it directly influences their chiroptical properties and potential utilities in advanced technologies. However, achieving reversible and dynamic manipulation of g lum in CP‐OURTP materials remains a formidable challenge. Herein, an effective strategy is presented to fabricate the chiral superstructure elastomers (CSEs) that display selective reflection colors, dynamically tunable CP‐OURTP with robust g lum values, full‐color afterglow emissions, and superior processability within a single system. By integrating room temperature phosphorescence (RTP) polymers into the CSEs, CSEs are produced demonstrating tunable CP‐OURTP with g lum values switching between 0.8 and 0.15 by mechanical deformation. More importantly, these mechanochromic, programmable, and full‐color CP‐OURTP films enable the development of flexible and dynamic information encryption and decryption. The work provides new insights into the development of novel RTP materials and advances in their potential applications.