A novel electrochemical separation process was developed to recover lithium from an end-of-life lithium-ion battery of an electric vehicle using an environmentally friendly and cost-effective process based on electrodialysis. Lithium, nickel, manganese, and cobalt were first extracted from the cathode material of a spent lithium-ion battery through a hydrometallurgical leaching process using H2SO4+H2O2 leachant under the optimal operating conditions. After leaching, nickel, manganese, and cobalt were recovered as complex anions coupled with ethylenediaminetetraacetic acid chelating agent, whereas lithium was recovered as lithium hydroxide using electrodialysis. The results showed that almost 100% of lithium was separated from nickel, manganese, and cobalt. Future work is underway to improve and optimize the separation process.