Layered double hydroxide-fullerene hybrid (LDH-C60) was facilely obtained via a co-precipitation method. Transmission electron micrographs (TEM), scanning electron micrographs (SEM), and X-ray photoelectron spectroscopy (XPS) all provided evidence that C60 was bound to LDH layers, resulting in a reduction in the size and thickness of the layer. Thermogravimetric analysis (TGA) and differential scanning calorimetry (DSC) findings indicated that LDH-C60 may greatly increase the thermal stability of PE. With the addition of LDH, the initial decomposition temperature (Tonset) of PE in N2 was lowered from 463 °C to 451 °C. The thermal stability of PE composites was increased with the addition of LDH-C60, though. For PE/LDH-C60 in N2 and air, the Tonset may be increased by 7 °C and 60 °C, respectively. Due to the interlayer water and anions' poor antioxygen capacity, the OIT for PE/LDH was also noticeably shorter than for PE. Furthermore, the OIT for PE/LDH-C60 was significantly delayed to 12.9 min. LDH-C60 shown a good synergistic impact in enhancing the thermal stability and anti‑oxygen capacity of polyethylene by combining the benefits of LDH and C60.