The ubiquitous manufacturing of lithium-ion batteries (LIBs) due to high consumer demand produces inevitable e-waste that imposes severe environmental and resource sustainability challenges. In this work, the charge storage capability and Li-ion kinetics of the recovered water-leached graphite (WG) anode from spent LIBs are enhanced by using an optimized amount of recycled graphene nanoflakes (GNFs) as an additive. The WG@GNF anode exhibits an initial discharge capacity of 400 mAh g-1 at 0.5C with 88.5% capacity retention over 300 cycles. Besides, it delivers an average discharge capacity of 320 mAh g-1 at 500 mA g-1 over 1000 cycles, which is 1.5-2 times higher than that of WG. The sharp increase in electrochemical performance is due to the synergistic effects of Li-ion intercalation into the graphite layers and Li-ion adsorption into the surface functionalities of GNF. Density functional theory calculations reveal the role of functionalization behind the superior voltage profile of WG@GNF. Besides, the unique morphology of spherical graphite particles trapping into graphene nanoflakes provides mechanical stability over long-term cycling. This work explains an efficient strategy to upgrade the electrochemical compatibility of recovered graphite anode from spent LIBs toward next-generation high-energy-density LIBs. © 2023 American Chemical Society.