During surface-enhanced fluorescence processes, the spatial spacing layer on the surface of noble metals plays an important role in regulating the fluorescence intensity. We propose a method for regulating fluorescence intensity using the AgNPs@TA-FeIII composite nanostructured materials as the substrate and using characteristic fluorescence of graphene quantum dots as the detection signal. Tannins-FeIII (TA-FeIII) nanofilms were prepared with a one-step assembly method, which is simple, fast, green, and safe. This work is expected to help the application of polyphenol metal nanofilm technology in the field of surface enhanced fluorescence (SEF).