In order to explore the method of large-scale industrial recycling and reuse of spent LiFePO4, regenerated LiFePO4/C material was synthesized by reducing and roasting spent LiFePO4 powder with carbon source. Furthermore, the effects of different carbon contents on the structure、morphology and electrochemical performance of regenerated LiFePO4 materials were investigated simultaneously by XRD, SEM and electrochemical measurements. The results show that the materials synthesized by reduction roasting by adding glucose, PEG and graphene combined carbon source to spent lithium iron phosphate powder all exhibited excellent performance in half-cells. The regenerated LiFePO4 cathode material delivered a discharge capacity of 162.7 mA·h/g at 0.1 C rate, and the capacity retention rate remained to be 95.53% after 100 cycles at 1 C rate. This method of regenerating LiFePO4 with simple operation, convenient preparation and low cost is a viable way to realize large-scale industrial recycling of spent LiFePO4.