Abstract <p>Graphite remains the most widely used anode material for lithium-ion batteries owing to its robust structure, low cost, and long-term cycling stability. However, spherical graphite often suffers from limited surface area, insufficient electrolyte wetting, and sluggish lithium-ion diffusion, which collectively restrict its rate capability and interfacial kinetics. A conformal carbon coating can mitigate these limitations by improving surface wettability, stabilizing the graphite–electrolyte interface, and providing additional pathways for fast charge transport. Nevertheless, many conventional carbon-coating approaches depend on organic solvents, raising concerns regarding sustainability and large-scale manufacturability. Herein, aqueous-based carbon-coating strategy is developed to address these limitations, which integrates thermal pretreatment, aqueous polyvinyl alcohol infiltration, iodine-assisted stabilization, and carbonization to produce an amorphous carbon layer that uniformly encapsulates spherical graphite particles. The resulting anode material achieves low charge-transfer resistance of 159 Ω, great reversible capacity over higher C-rates, and maintains a discharge capacity of 203 mAh g⁻¹ at 5 C, outperforming pristine spherical graphite. The sustainable aqueous method underscores the potential for scalable and environmentally responsible manufacturing of improved graphite anodes. It is believed that these insights provide valuable design principles for future research on sustainable strategies.</p> Graphical abstract