Water Radiolysis Enables CO ₂ ‐Activated Radical Recycling of Spent Lithium‐Ion Cathodes

ABSTRACT Conventional recycling of spent lithium‐ion batteries (LIBs) relies on energy‐intensive and complex processes that hinder sustainability. Here, we report a mild, efficient recycling strategy using programmable water radiolysis with CO 2 to establish an aqueous reductive radical platform. This radiolytic approach enables simultaneous cathode peeling, metal leaching, and component separation under ambient conditions, which is inaccessible to existing methods. Within minutes, high‐dose‐rate irradiation degrades the polymeric binder, enabling ∼99.5% active material recovery. Radiolytically generated CO 2 •− radicals reduce and leach transition metals (Co, Ni, Mn) and lithium with >96% efficiency. The dynamic pH evolution during irradiation precipitates transition metals in situ as carbonates while retaining Li + in solution, accomplishing one‐step separation. Regenerated cathodes deliver electrochemical performance comparable to commercial benchmarks. Techno‐economic analysis indicates this CO 2 ‐mediated radiolytic pathway offers a more sustainable, energy‐efficient, and cost‐effective route for battery recycling.