Renewable energy and electric vehicles are well-acknowledged strategies for reducing CO 2 emissions, and their development relies heavily on the core of energy storage systems using lithium-ion batteries. However, recycling of lithium-ion batteries is far from mature, and massive abandonment of spent batteries would lead to severe environmental pollution. Meanwhile, the shortage of lithium resources brought about by the rapid development of lithium-ion batteries, especially LiFePO 4 , significantly drives up the preparation cost of Li 4 SiO 4 as a promise sorbent and greatly limits its application as a CO 2 capture scheme. Hence, a strategy is urgently needed to alleviate the lithium resource contradiction between energy storage and CO 2 mitigation. Herein, we report a novel concept in recycling spent LiFePO 4 battery to prepare high-efficiency and low-cost Li 4 SiO 4 sorbents for CO 2 capture. The obtained Li 4 SiO 4 sorbents demonstrate very stable CO 2 capacities of 0.27− 0.28 g/g in a typical test up to 80 cycles, a leading level in CO 2 capture, while the cost is only 1/6 of the conventional preparation process. It suggests that the concept of recycling spent LiFePO 4 for CO 2 capture has broad implications on resource utilization of energy waste and the mitigation of CO 2 emissions. KEYWORDS: CO 2 adsorption, spent lithium-ion battery, Li 4 SiO 4 , high-temperature CO 2 sorbent