High-capacity anode materials are promising candidates for increasing the energy density of lithium (Li)-ion batteries due to their high theoretical capacities. However, a rapid capacity fading due to the huge volume changes during charge-discharge cycles limits practical applications. Herein, a layering-charged polymeric binder is introduced that can effectively integrate high-capacity anodes using a strong yet reversible Coulomb interaction and enriched hydrogen bonding. The charged polymeric binder builds a dynamically charge-directed network on the active materials with high versatility and efficiently dissipates the electrode stress with its excellent mechanical properties. Such an unprecedented charge-directed binder pro-vides insights into the rational design of a binder for high-capacity anodes.