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Polymer binders are critical auxiliary additives to Li-ion batteries that provide adhesion and cohesion for electrodes to maintain conductive networks upon charge/discharge processes. Therefore, polymer binders become interconnected electrode structures affecting electrochemical performances, especially in LiFePO₄ cathodes with one-dimensional Li⁺ channels. In this paper, recent improvements in the polymer binders used in the LiFePO₄ cathodes of Li-ion batteries are reviewed in terms of structural design, synthetic methods, and working mechanisms. The polymer binders were classified into three types depending on their effects on the performances of LiFePO₄ cathodes. The first consisted of PVDF and related composites, and the second relied on waterborne and conductive binders. Profound insights into the ability of binder structures to enhance cathode performance were discovered. Overcoming the bottleneck shortage originating from olivine structure LiFePO₄ using efficient polymer structures is discussed. We forecast design principles for the polymer binders used in the high-performance LiFePO₄ cathodes of Li-ion batteries. Finally, perspectives on the application of future binder designs for electrodes with poor conductivity are presented to provide possible design directions for chemical structures.