Abstract: An electrode for an electrochemical energy storage device includes an electrode active material and a crosslinked binder. The crosslinked binder includes a polyelectrolyte composed of monomer units, wherein at least a portion of the monomer units has at least one carboxyl group per unit, and a crosslinking agent, wherein the polyelectrolyte is crosslinked by the crosslinking agent. The crosslinking agent is selected from a polyphosphate and a combination of ethylenedinitrilotetraacetic acid (EDTA) with sodium ions. The electrode active material is held together by the crosslinked binder. Further provided are methods for forming the electrode, electrode slurries comprising the crosslinked binder, and electrochemical energy storage devices that employ the electrode as an anode, a cathode, or both.