Recycling lithium and graphite from spent lithium-ion battery plays a significant role in mitigation of lithium resources shortage, comprehensive utilization of spent anode graphite and environmental protection. In this study, spent graphite was firstly collected by a two-stage calcination. Secondly, under the optimal conditions of 1.5 M HCI, 60 min and solid-liquid ratio (S/L) of 100 g·L−1, the collected graphite suffers simple acid leaching to make almost 100% lithium, copper and aluminum in it into leach liquor. Thirdly, 99.9% aluminum and 99.9% copper were removed from leach liquor by adjusting pH first to 7 and then to 9, and thenthe lithium was recovered by adding sodium carbonate in leach liquor to form lithium carbonate with high purity (>99%). The regenerated graphite is found to have high initial specific capacity at the rate of 37.2 mA·g−1 (591 mAh·g−1), 74.4 mA·g−1 (510 mAh·g−1) and 186 mA·g−1 (335 mAh·g−1), and with the high retention ratio of 97.9% after 100 cycles, it also displays excellent cycle performance at high rate of 372 mA·g−1. By this process, copper and lithium can be recovered and graphite can be regenerated, serving as a sustainable approach for the comprehensive utilization of anode material from spent lithium-ion battery.