In this work, a core-shell hierarchical LiFe5O8@PPy nanocomposite has been successfully fabricated through a simple etching/regrowing method. The core buffer of highly conducive PPy nanotubes is introduced to enhance the electrochemical performance of LiFe5O8. Owing to improved electron transfer capability, charge transfer resistances of the core-shell nanostructured composites are decreased and the electrochemical properties are enhanced. The representative LiFe5O8@PPy nanocomposite exhibits a high specific capacitance of 292 F g(-1) at a scan rate of 5 mV s(-1), and an excellent cycling stability (82.99% after 10,000 cycles) because of the synergistic effect of LiFe5O8 nanosheets and PPy nanotubes. This study confirms that the as-prepared LiFe5O8@PPy nanocomposites are promising candidates for supercapacitor electrode materials.