Advancing electrode materials with high adsorption capacity and fast rate is crucial for seawater desalination in capacitive deionization (CDI).Here, we propose a highly oriented, densified graphene (HODG) electrode characterized by its ordered/short ion transport channels, abundant oxygen functional groups, high packing density (1.374 g cm −3 ), and large specific surface area (543.72 m 2 g −1 ), facilitating exceptional fast ion diffusion and ultrahigh volumetric desalination capacity. HODG delivers a volumetric capacitance of 308 F cm −3 at 1 A g −1 , and a record-high volumetric salt adsorption capacity (v-SAC) of 57.70 mg cm −3 with a rapid rate of 1.92 mg cm −3 min −1 at 1.2 V in 1000 mg L −1 NaCl. Even after 50 cycles of adsorption−desorption, it can still retain 91.36% of its initial desalination capacity. This proposed design strategy offers a new avenue for the rational optimization of graphene architectures, boosting the development of high-performance CDI electrode materials toward practical applications.