Dynamic Hydrogen Bonding Enables Room‐Temperature Phosphorescent Films with Multi‐Stimuli Responsiveness and Remodelability for Rewritable Pattern Display

Abstract With the growing demand for dynamic pattern display, stimulus‐responsive room‐temperature phosphorescence (RTP) materials are highly desirable. However, achieving tunable responsive phosphorescence and excellent remodelability in such materials remains challenging due to their intricate photophysical processes. Herein, a dynamic hydrogen bonding strategy is leveraged to develop stimulus‐responsive RTP films with shape malleability by incorporating naphthylamide‐grafted polydimethylsiloxane into the polyacrylic acid (PAA) matrix. The incompatibility between the polydimethylsiloxane with different chain lengths and the PAA network leads to a controllable phase‐separated structure, enabling the regulation of phosphorescence performance of the films. Notably, the dissociation of hydrogen bonds between polymer networks upon exposure to high humidity or increased temperature imparts the films with excellent stimuli‐responsive phosphorescence. Particularly, the difference in hydrophobic siloxane chains affects luminescence color‐changing rates under the trigger of humidity. Moreover, the reversibility of the hydrogen bond allows for luminescent rewritability through an alternating water diffusion/evaporation process. Impressively, the shape malleability of the films is achieved without compromising their phosphorescence behavior owing to dynamic hydrogen bonding. Ultimately, a shape‐remodeling intelligent platform with rewritability is demonstrated to dynamically display information. This study provides a reliable approach to designing stimulus‐responsive RTP materials through dynamic interaction and expands their applications in environmentally friendly pattern display.