A self-healing supramolecular polymer composite (LP-GO) is designed and prepared via incorporation of graphene oxide (GO) to hyperbranched polymer by hydrogen-bonding interactions. The polymer matrix based on amino-terminated hyperbranched polymer is synthesized by dimer acid and diethylene triamine, while GO is prepared by the modified Hummers method. Infrared spectroscopy (FTIR), thermo gravimetric testing (TGA), X-ray diffraction (XRD), and scanning electron microscopy (SEM) is applied to characterize GO. Stressstrain test is utilized to characterize the obtained self-healing property of LP-GO. It is found that just a small amount of GO (up to 3 wt %) is needed to achieve a dramatic improvement in the mechanical properties, and self-healing efficiency of the polymer composites. After healing at 60 oC for 1 h, the addition of GO even restores the self-healing efficiency to 100% of its original tensile strength. In striking contrast to conventional cross-linked or thermoreversible rubbers made of macromolecules, these systems, when being broken or cut, can be simply healed by contacting fractured areas again to self-heal at suitable temperature. Building on the unique self-healing properties, the simplicity of synthesis and the availability from renewable resources, etc., LP-GO bodes well for broader applications in the near future.