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The development of lithium-ion batteries (LIBs) is important in the realm of energy storage. Understanding the intricate effects of binders on the Li⁺ transport at the cathode/electrolyte interface in LIBs remains a challenge. This study utilized molecular dynamics simulations to compare the molecular effects of conventional polyvinylidene difluoride (PVDF), Li⁺-coordinating polyethylene oxide (PEO), and negatively charged polystyrene sulfonate (PSS) binders on local Li⁺ mobility at the electrolyte/LiFePO₄ (LFP) cathode interface. By examining concentration profiles of Li⁺, three different polymer binders, and anions near Li⁺-rich LFP and Li⁺-depleted FePO₄ (FP) surfaces, we found a superior performance of the negatively charged PSS on enhancing Li⁺ distribution near the Li⁺-depleted FP surface. The radial distribution function and coordination number analyses revealed the potent interactions of PEO and PSS with Li⁺ disrupting Li⁺ coordination with electrolyte solvents. Our simulations also revealed the effects of non-uniform binder dispersions on the Li⁺ local mobility near the cathode surface. The combined results provide a comparative insight into Li⁺ transport at the electrolyte/cathode interface influenced by distinct binder chemistries, offering a profound understanding of the binder designs for high-performance LIBs.