In parallel to the depletion of potable water reservoirs, novel technologies have been developed for seawater softening, as it is the most abundant source for generating deionized water. Although salt removal at subosmotic pressures and ambient temperatures by applying low-operating potentials with high energy efficiency made capacitive deionization (CDI) an advantageous water-softening process, its practical application is limited by insufficient ion removal capacity and low concentration influent. The performance of a CDI system is in progress with engineering the electrode active materials, also facilitating the advance design in highly saline-and seawater study. Herein, an innovative strategy was developed to provide high-performance CDI systems based on efficient and electrochemical ion-uptake active materials with a simple initial preparation. Nitrogen-doped porous carbons (N-pCs) received benefits from a high specific surface area and good surface wettability. The N-pCs were modified with molybdenum oxide/sulfide intercalative array and developed as CDI electrode active materials for desalination of both low/medium saline-and seawater. The MoS 2 /S,N-pC electrode materials exhibited perfect optimized salt adsorption capacity (SACs) of 47.9 mg g −1 when compared to N-pC (37.9 mg g −1 ) and MoO 3 /N-pC (39.6 mg g −1 ) counterparts at 1.4 V in a 750 ppm NaCl solution. In addition, the assembled CDI cells exhibited reasonable cycle stability and retained 96.7% of their initial SAC in continuous CDI cycles for 128,000 s. The fabricated CDI cell rendered an excellent salt removal efficiency (SRE, %) of 13.34% from the real seawater sample at 1.2 V. In detail, the SRE % of the NaCl, KCl, MgCl 2 , and CaCl 2 soluble salts with respect to seawater sample exhibited a remarkable SRE % of 30.8%, 36%, 32.6%, and 19.3%, respectively. These SRE % values (>13.34%) provide convincing evidence on the reasonable ion uptake capability of the fabricated CDI cells for removing Na + , K + , Mg 2+ , and Ca 2+ ions compared to other soluble component. The advanced cell design parallel to the promising outcomes provided herein makes these CDI systems immensely propitious for efficient water softening.