With the environmental pollution and shortage of resources, the recycling and reusing of spent lithium-ion batteries become crucial. However, the complexity of recycling methods, associated with high cost, makes their recovery difficult. Herein, an effective and clean process to recycle anode materials from lithium-ion batteries and reuse graphite is proposed in this work. The graphite and copper foil of the anode are separated by electrolysis method, and the effects of parameters (voltages, inter-electrode distance, and electrolyte concentration) on the electrolysis process are investigated. The copper foil can be directly reused without further treatment, Cu2+ and Li+ in the electrolyte can be recovered by precipitation method. The purity of recovered graphite is about 95%, and the graphite can be reused to prepare the anode materials for lithium-ion batteries that exhibit excellent cycling stability and rate capability. The first discharge and charge specific capacities at a rate of 0.1 C are 427.81 mA h g−1 and 350.47 mA h g−1, respectively. The coulombic efficiency after the second cycle is observed to be about 98%.