The graphene oxide (GO)-based fluoropolymer is first proposed as an interface encapsulant to improve the light extraction efficiency and achieve the ultralong working stability of deep ultraviolet light-emitting diodes (DUV-LEDs), benefitting from its superior interface performance based on an anchored effect. For the GO-based fluoropolymer composite, the anchored structure is designed to effectively and tightly rivet the quartz lens on the DUV-LED chip by using the interface reaction between GO embedded in fluoropolymer and 3-aminopropyltriethoxy-silane grafted on the surfaces. Experimental results show that on the basis of the interface anchored effect, the air voids in the interface layer of DUV-LED are reduced by 84%, leading to an improvement of the light output power by 15% and a decrease of the junction temperature by 5%, by virtue of the sealing characteristics of the 0.10 wt % GO-based fluoropolymer. In addition, the steady working time is dramatically improved by 660% and it was attributed to the good interface anchored bonding of the 0.10 wt % GO-based fluoropolymer. This novel graphene oxide-based fluoropolymer is believed to provide a feasible and effective interface encapsulant to improve the performance of DUV-LEDs.