Li, Fe and V were reclaimed together and preparedSto xLiFePO₄-yLi₃V₂(PO₄)₃ materials from spent LiFePO₄ and Li₃V₂(PO₄)₃ LIBs, for the reason that they have similar characteristics and preparation method. The spent battery materials were roasted under 600 _oC for 1 hour in air atmosphere to remove the PVDF binder, then the active materials and aluminum foil collector can be separated effectively. The different proportion of xLiFePO₄-yLi₃V₂(PO₄)₃(x:y=5:1,7:1,9:1) materials were prepared by roasted products through adjusting the mole ratio of Li, Fe, V and P , ball milling and calcining. The morphology, structure and electrochemical of composite material were performed. The results show that the composite material have the electrochemical properties of LiFePO₄ and Li₃V₂(PO₄)₃ simultaneously, which can significantly improve the LiFePO₄ ratio performance. This dissertation explores a new way for the recycling of spent LIBs. The study is of good application foreground. It is very important for environmental protection, and is believed to bring both economic and social benefits to us.