Responsive luminescent materials that reversibly

react to external stimuli have emerged as prospective platforms for

information encryption applications. Despite brilliant achieve-

ments, the existing fluorescent materials usually have low

information density and experience inevitable information loss

when subjected to mechanical damage. Here, inspired by the

hierarchical nanostructure of fluorescent proteins in jellyfish, we

propose a self-healable, photoresponsive luminescent elastomer

based on dynamic interface-anchored borate nanoassemblies for

smart dual-model encryption. The rigid cyclodextrin molecule

restricts the movement of the guest fluorescent molecules, enabling

long room-temperature phosphorescence (0.37 s) and excitation

wavelength-responsive fluorescence. The building of reversible

interfacial bonding between nanoassemblies and polymer matrix together with their nanoconfinement effect endows the

nanocomposites with excellent mechanical performances (tensile strength of 15.8 MPa) and superior mechanical and functional

recovery capacities after damage. Such supramolecular nanoassemblies with dynamic nanoconfinement and interfaces enable

simultaneous material functionalization and self-healing, paving the way for the development of advanced functional materials.