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A polyvinylpyrrolidone (PVP)-based fluorescent film with stable optical properties is successfully prepared in one pot without any additive.The reaction mechanism of ring-opening and self-crosslinking of linear PVP is proposed and demonstrated by NMR spectra.The morphologies and the structures of the fluorescent film as well as the blank film are investigated.Emission spectra and X-ray diffraction pattern of the PVP-based fluorescent film illustrates that dye is incorporated into the film networks via covalent linkages, thus leading to the highly stable optical properties.The facile and effective synthesis approach opens a new way for the design of other multi-functional composite materials based on PVP.