Unlocking High‐Capacity Graphite Cathode in Dual‐Ion Batteries Through Structural Disorder Regulation

Dual‐ion batteries (DIBs) represent a transformative platform in energy storage applications, owing to their exceptional capability to operate at elevated voltages (above 5.0 V) while maintaining a low production cost. However, their actual capacity is severely limited by the anion‐only intercalation in conventional graphite cathodes. Here, we present a graphite cathode featuring multiscale disordered architectures (SDG‐800), achieved via a one‐step yet multifunctional pyrolysis strategy to simultaneously realize the low‐temperature catalytic graphitization with controlled vacancy defects, the formation of micropores, and the doping of heteroatoms. The unique architectures of SDG‐800 serve as a platform for synergistic ion reservoirs, effectively activating multi‐mode ion co‐storage mechanisms within a single electrode. When integrated into a DIB, the SDG‐800 cathode exhibits a record‐breaking capacity of 264 mAh g −1 (representing a 2.4‐fold enhancement over conventional graphite), coupled with an impressive energy density of 648 Wh kg − 1 and a long cycling durability exceeding 1400 cycles. This work provides an innovative design strategy for graphite‐based cathodes in high‐performance DIB systems.