A Dynamic H‐Bonding Network Enables Stimuli‐Responsive Color‐Tunable Chiral Afterglow Polymer for 4D Encryption

Abstract The development of stimuli‐responsive and color‐tunable chiral organic afterglow materials has attracted great attention but remains a daunting challenge. Here, a simple yet effective strategy through the construction of a dynamic H‐bonding network is proposed to explore the multi‐color stimuli‐responsive chiral afterglow by doping a self‐designed chiral phosphorescent chromophore into a polyvinyl alcohol matrix. A stimuli‐responsive deep blue chiral afterglow system with a lifetime of up to 3.35 s, quantum yield of 25.0%, and luminescent dissymmetry factor of up to 0.05 is achieved through reversible formation and breakdown of the H‐bonding network upon thermal‐heating and water‐fumigating. Moreover, multi‐color stimuli‐responsive chiral afterglow can be obtained by chiral and afterglow energy transfer, allowing the establishment of afterglow information displays and high‐level 4D encryption. This work not only offers a facile platform to develop advanced stimuli‐responsive materials but also opens a new avenue for developing next‐generation optical information technology with enhanced functionality and responsiveness.