Non-traditional luminescent polymers exhibit significant advantages in biodiagnostics and intelligent materials but suffer from low luminescence efficiency and limited functionality. Inspired by the excited-state proton transfer mechanism mediated by dense hydrogen bonds in jellyfish fluorescent proteins,we propose a strategy using dynamic quadruple hydrogen bonding ureidopyrimidinone motifs to create highly efficient luminescent polymers. By modulating the aggregated structure of the supramolecular units, proton transfer between paired motifs is activated, thereby achieving a high photoluminescent

quantum yield up to 52% in supramolecular polyurethane. Ultrafast spectroscopy directly revealed this intermolecular proton transfer, while solid-state NMR spectroscopy confirmed the essential role of quadruple hydrogen bonds. The dynamically switchable hydrogen bonding structure endows the material with multifunctional integration, including strong fluorescence properties, high toughness, self-healing, reprocessability, and stimulus responsiveness. This research not only introduces a pioneering approach for advancing high-performance light-emitting materials but also enhances the prospects for their practical applications.