Zhiheng Zhou, Xinzhen Fan, Chuanzhuang Zhao
Abstract A critical challenge in multifunctional room‐temperature phosphorescent (RTP) hydrogels is the balance between the persistent afterglow and the editable phosphorescent information. Inspired by the Hawaiian bobtail squid ( Euprymna scolopes ), which modulates bioluminescence through symbiotic bacterial storage and release, a biomimetic RTP hydrogel system is introduced that overcomes this limitation. The hydrogel, synthesized via polymerization of acrylic acid (AA) with diethylenetriamine (DETA), followed by Ca 2+ coordination with COO − in polyacrylic acid (PAA) chains, exhibits remarkable phosphorescence (afterglow > 6.5 s) and three synergistic functionalities: 1) Dynamic information re‐editability via water erasing and salt printing for real‐time information programming; 2) Thermomechanical responsiveness enabling reversible stiffness modulation and thermal concealment of photonic information; 3) Self‐healing through dynamic hydrogen bonding, facilitating dynamic reconfiguration of luminescent patterns. This RTP hydrogel establishes a robust platform for the edition of information, which emphasizes the potential of bioinspired strategies for advancing intelligent materials in bioimaging, flexible displayers, and information encryption.