Abstract The utilization of polymeric binders is indispensable in the implementation of silicon/carbon anode materials in high-energy-density lithium-ion batteries (LIBs). This necessity arises from their pivotal function in upholding structural integrity. However, current water-based binders solely focus on binder adhesion, neglecting the crucial interaction with the carbon material. In this work, a composite binder (CMC-CPAM-SBR) was constructed by combining Styrene Butadiene Rubber (SBR) with cationic polyacrylamide (CPAM) network binder with self-healing carboxymethyl cellulose (CMC). This innovative binder formulation was designed to enhance the performance of Si@C/graphite composite anodes. A capacity retention rate of 92.86% was achieved after 100 cycles, which represents the improvement over the performance of electrodes utilizing the CMC-CPAM binder, which only retained a capacity of 84.53% after the same number of cycles. A full battery with a capacity of 1992.8 mAh was designed, and the battery capacity remained at 80.6% of its capacity after completing 500 cycles. This research presents an effective technique for manufacturing high-performance anode materials.