Capacitive deionization (CDI) is a promising desalination technology because of its simple, high energy efficient, and eco-friendly process. Among several factors that can affect the desalination capacitance of CDI, wettability of the electrode is considered one of the important parameters. However, various carbon materials commonly have a hydrophobic behavior that disturbs the ion transfer between the bulk solution and the surface of the electrode. In this study, we fabricated a layered double hydroxide (LDH) coated activated carbon electrode using an in-situ growth method to enhance the wettability of the surface of the carbon electrode. The well-oriented and porous LDH layer resulted in a better wettability of the activated carbon electrode, attributing to an enhanced capacitance compared with that of the uncoated activated carbon electrode. Furthermore, from the desalination tests of the CDI system, the LDH coated carbon electrode showed a higher salt adsorption capacity (13.9 mg/g) than the uncoated carbon electrode (11.7 mg/g). Thus, this enhanced desalination performance suggests that the improvement in the wettability of the carbon electrode by the LDH coating provides facile ion transfer between the electrode and electrolyte.