With the increasing popularity of new energy electric vehicles, the demand for lithium-ion batteries (LIBs) has been growing rapidly, which will produce a large number of spent LIBs. Therefore, recycling of spent LIBs has become an urgent task to be solved, otherwise it will inevitably lead to serious environmental pollution. Herein, a unique recycling strategy is proposed to achieve the concurrent reuse of cathode and anode in the spent graphite/LiFePO4 batteries. Along with such recycling process, a unique cathode composed of recycled LFP/graphite (RLFPG) with cation/anion-co-storage ability is designed for new-type dual-ion battery (DIB). As a result, the recycle-derived DIB of Li/RLFPG is established with good electrochemical performance, such as an initial discharge capacity of 117.4 mA h g−1 at 25 mA g−1 and 78% capacity retention after 1000 cycles at 100 mA g−1. The working mechanism of Li/RLFPG DIB is also revealed via in situ X-ray diffraction and electrode kinetics studies. This work not only presents a far-reaching significance for large-scale recycling of spent LIBs in the future, but also proposed a sustainable and economical method to design new-type secondary batteries as recycling of spent LIBs.