Capacitive deionization techniques are of interest in water treatment technology due to their low cost, excellent efficiency, and environmental friendliness. Currently, metal–organic frameworks are highly impactful candidates for use as electrode materials in electrochemistry. It provides a large pore volume, good chemical stability, and a high specific surface area. Tuning metal–organic frameworks with carbon materials will have a good impact on electrode materials with increasing performance. This study shows a facile and effective strategy for arranging flow capacitive desalination technology for salt removal. The conducting network of Fe-MOF/CNTs provides rapid electron transport and offers a high diffusion length of ions. This material exhibited excellent desalination performance, with a high salt adsorption of 80.575 mg/g at 1.6 V at an initial NaCl concentration of 1000 mg/L. Overall, the facile method and fabrication strategy greatly advances water treatment applications.