Abstract: Lithium iron phosphate (LiFePO4, LFP) is a widely adopted cathode material in lithium-ion batteries due to its intrinsic thermal stability, safety, and long cycle life. However, repeated charging and discharging cycles cause the lithium depletion (delithiation) and structure degradation, ultimately resulting in diminished battery performance and the accumulation of spent battery wastes. Conventional recycling methods, such as pyrometallurgy and hydrometallurgy, present significant limitations: pyrometallurgical processes are energy-intensive due to high-temperature smelting, while hydrometallurgical approaches rely on corrosive reagents and involve complex separation steps to recover high-purity precursors. Although effective in the short term, these methods are not conducive to achieving a closed-loop, environmentally sustainable battery economy. In this study, we explore a direct regeneration strategy for the recovery of spent LiFePO4. This approach restores the electrochemical activity of the degraded material via relithiation and defect restoration, without disrupting its original crystal structure. Our findings show that approximately 70% of the original electrochemical performance can be restored through this method, highlighting its potential as a cost-effective and sustainable solution for lithium-ion battery recycling.