Wavelength‐Gated Spatiotemporal Phosphorescent Reconfiguration with Protein Aggregation‐Enabled Unclonability

ABSTRACT Dynamic room‐temperature phosphorescence (RTP) and physical unclonable function (PUF) represent promising anti‐counterfeiting approaches. However, significant challenges remain in achieving their synergistic integration within a single‐material system while maximizing the respective advantages of both functionalities. In this study, a time‐dependent phosphorescent color‐tuning platform based on flexible protein film is proposed, and the dynamic reconstruction of optical patterns in a single material system is realized by spatially selective dual‐emitter (1‐pyrenecarboxylic acid and lanthanide‐organic framework) doping for the first time. Specifically, the film exhibits a dual‐mode response of excitation wavelength selection, enabling rapid shape and color switching between two emitter‐dominated emission patterns, accompanied by progressive phosphorescent chromatic evolution from red → orange → yellow → green. In addition, through a controlled randomness strategy of coordinated control of solvent ratio and temperature substantially, the uncertainty aggregation in the protein self‐assembly process is adjusted into batch consistency, which significantly enhances label robustness and production yield. The synergistic integration of wavelength‐dependent dynamic responses and intrinsic physical unclonability establishes a new paradigm for high‐security anti‐counterfeiting, featuring unpredictability and multidimensional dynamic authentication.