Background <p>Silicon anodes possess an exceptionally high theoretical capacity, rendering them promising candidates for next-generation lithium-ion batteries, while their practical deployment is severely hindered by pronounced mechanical degradation during cycling. Polymer binders are essential for maintaining electrode integrity, yet their mechanical roles are typically assessed using limited descriptors, obscuring the complex coupling between binder mechanics and electrochemical performance.</p> Objective <p>This study aims to establish a multidimensional mechanical-electrochemical framework to quantitatively elucidate how binder mechanical properties govern the cycling stability of silicon electrodes.</p> Methods <p>Eight representative binders with diverse molecular architectures were systematically characterized in terms of elastic modulus, ultimate strength, fracture elongation, fracture toughness, adhesive strength, and fatigue resistance. These properties were then correlated with the electrochemical performance of electrodes using Sobol sensitivity analysis.</p> Results <p>The results identify adhesive strength as the dominant mechanical factor controlling the cycling performance of silicon electrodes. Additionally, Pearson correlation analysis reveals an inherent trade-off between stiffness/adhesion and deformability/toughness, leading to two fundamental binder archetypes: structural-constraint and deformation-adaptive binders.</p> Conclusions <p>This study provides a quantitative, mechanics-based understanding of binder functionality and offers design principles for advanced binders that enable durable, high-performance silicon electrodes.</p>