Zinc-Metal Batteries In article number 2401610, Jin Gu Kang, Dong-Wan Kim, and co-workers introduced an ionically cross-linked composite hydrogel for modulating the electrical double layer on Zn metal anodes. To achieve long-lasting zinc-metal batteries, a molecularly engineered hydrogel layer is introduced to modulate the electrical double layer (EDL) at the anode interface. By repelling water and sulfate ions, the layer suppresses corrosion and side reactions, promoting uniform, dendrite-free zinc growth. This strategic EDL control ensures exceptional durability and an extended battery lifespan.