The rising demand for lithium, with its central role in energy storage device, have raised emphasis on lithium recovery from alternative and untapped lithium sources, such as from spent lithium ion batteries (LIBs). Lithium recovery from spent LIBs via pyrometallurgical and hydrometallurgical methods typically demands substantial energy and chemical inputs, and suffers from lithium losses during multi-step separations. Here, we introduce a redox-active, lithium-selective polymer that enables highly selective, acid-free, and energy-efficient lithium recovery from spent LIB leachates. The copolymer combines a lithium-binding ligand with a redox-active ferrocene moiety, allowing lithium uptake in non-aqueous media and its electrochemically-driven release through ferrocene oxidation. Additionally, electrochemical activation enhances lithium uptake kinetics by reducing mass transport barriers at the polymer–electrolyte interface. The system exhibits remarkable lithium uptake across various organic solvents, including those commonly used in LIB electrolytes (dimethyl carbonate and propylene carbonate) and leaching processes (N-methyl-2-pyrrolidone). Selective lithium capture is demonstrated from cathode, anode, and separator leachates of both lithium nickel manganese cobalt and lithium iron phosphate batteries. Long-term cycling stability and techno-economic analysis further validate the robustness and cost-effectiveness of this redox-mediated recovery platform. Overall, this work establishes a new design framework for electrifying selective adsorbents, providing a sustainable and scalable approach for critical metal recovery.
