Traditional polymeric binders (Li-PAA, CMC, etc.) are partly capable of sustaining the large volumetric variation of high-capacity anodes during battery operation which potentially replace low-capacity graphite. However, insufficient bond strength and poor reversibility of the binder network lose initial structure and eventually fail. In this presentation, directed coacervation based on the charged polymers will be introduced into the binder for high-capacity anodes in lithium-ion batteries. Layered-charged polymers along with negatively charged active materials form strong and reversible junctions in an electrolyte-infiltrated state. As a result, electrode integrity and ionic conduction were improved to extend a battery cycle life and formulate an ultrathick electrode.