As silicon content increases, electrical connectivity within the electrode becomes increasingly dependent on the structural stability of the carbon–binder domain (CBD). The viscoelastic CBD network exhibits incomplete elastic recovery during cycling, leading to interfacial gaps with silicon and the disruption of electrical pathways. These polymer-particle network originate during slurry process and are reflected in rheological responses. In this study, a new approach that correlates slurry viscoelasticity with cell performance to provide insights for improving the structural stability of high-silicon content anodes.