Capacitive deionization (CDI) is considered one of the most promising desalination technologies for obtaining fresh water from saline water. In this work, we synthesized a hollow core-shell Co-MOF@Fe/Co-LDH (Co-Fe-LDH) material by developing a strategy to simultaneously grow Co/Fe-LDH on the surface of a Co-MOF precursor in situ. Owing to the increase in the specific surface area of the hollow structure and the Faradaic process of a layered double hydroxide (LDH), the Co-Fe-LDH material exhibits high electrical double layer (EDL) capacitance and pseudocapacitance, which significantly improves the salt adsorption of the material during CDI (34.2 mg/g in a 600 mg/L NaCl solution at 1.2 V). The adsorption for NaCl in this work is approximately 2.5 times the maximum salt adsorption capacity (SAC) of LDH materials applied in nonmembrane CDI (NMCDI). This work may provide a promising model for the application of hollow LDH materials that exhibit pseudocapacitance in CDI. (C) 2020 Elsevier Inc. All rights reserved.