Direct recycling offers a promising alternative for regenerating spent Li‐ion batteries (LIBs); however, achieving high‐purity cathode and ensuring cost‐effectiveness remains challenging. Herein, we present an innovative integrated process that simultaneously enables delamination and relithiation of spent cathodes, Li _x Ni _0.6 Co _0.2 Mn _0.2 O ₂ and Li _x FePO ₄ , under open‐air conditions with minimal energy. By oxidizing diethylene glycol, a green solvent, the transition‐metal oxidation state in the cathode is effectively reduced, thereby facilitating Li reinsertion into the structure. Consequently, the formation of glycol aldehyde induces 100% electrode delamination, enabling a one‐pot restoration pathway. The reaction mechanism is elucidated using Proton nuclear magnetic resonance ( ¹ H‐NMR), Soft X‐ray absorption spectroscopy (soft‐XAS), and X‐ray absorption near‐edge structure spectroscopy (XANES), and the regenerated cathodes consistently recover over 99% of their electrochemical performance for both 2 and 50 Ah cells. Furthermore, the regeneration solution is reusable, requiring only Li salt supplementation. This study presents a practical, low‐cost, and environmentally friendly approach for advancing the scalability and feasibility of direct LIB recycling technologies.

Lithium–sulfur (Li-S) batteries are attractive next-generation energy storage systems owing to their high theoretical energy density of 2600 Wh/kg and earth-abundant, eco-friendly sulfur. However, their practical application is hindered by the insulating nature of sulfur, large volume changes during cycling, and the polysulfide shuttle effect. Herein, we designed a dual-confinement cathode architecture combining mesoporous carbon with earth-abundant titanium dioxide (TiO₂). Sulfur composites with 70 wt% sulfur loading were prepared. Structural characterization via X-ray diffraction (XRD) and Brunauer–Emmett–Teller (BET) analysis showed a well-developed mesoporous network in KB but not in TiO₂. XRD confirmed that sulfur and anatase TiO₂ coexist in the composites, with weaker sulfur peaks in the mixed host. UV-vis absorption spectra showed that nano-TiO₂ removes more Li₂S₆ from solution than KB. Electrochemical evaluations revealed that the dual-confinement composite architecture balances the fast redox kinetics of carbon against the polysulfide affinity of TiO₂. Consequently, the composite achieved a high initial discharge capacity of 1300.89 mAh/g at 0.1 C and stable cycling over 100 cycles at 0.5 C. Furthermore, ex situ XRD analysis revealed nearly complete sulfur conversion while maintaining TiO₂ structural integrity. These results demonstrate an optimal balance between electronic conductivity and polysulfide mitigation via a sustainable material strategy.