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[Display omitted] • Graphene oxide (GO) was attach on the carbon fiber (CF) surface, and the hybrid GO@CF was further alkylated to modulate the LLPDE/CF interface. • LLDPE/MGO@CF exhibit excellent mechanical and electrothermal functional properties. • The structural self-monitoring of LLDPE/MGO@CF composite could be reflected by the in-situ electrical resistance change. The rational modulation for the interfaces of polymer/filler composites is the key to maximizing its mechanical property and functional performance. In this work, the interface of recycled carbon fiber (CF) enhanced linear low-density polyethylene (LLDPE) composites was modulated via graphene oxide (GO) bridging and alkyl group modification to increase the interface roughness and improve the compatibility. The optimized composite displays improved mechanical, thermal, and electrical properties due to the modulated interface synergistic effect, particularly as a flexible heater, the composites film displayed excellent electrical heating behavior at a fast speed of heating up in 50 s to a steady-state temperature of 40 °C under the low voltage of 5 V. In addition, the structural self-monitoring of this conductive composite could be reflected by the electrical resistance change based on the results of finite element analysis (FEA) and in-situ resistance-tensile measurements. This facile compatibilization approach and in-situ self-monitoring method provide a new route for expanding the application of functional polyethylene materials. [ABSTRACT FROM AUTHOR]