This work establishes molybdenum disulfide/carbon nanotube electrodes for the desalination of high molar saline water. Capitalizing on the two-dimensional layered structure of MoS2, both cations and anions can be effectively removed from a feed water stream by faradaic ion intercalation. The approach is based on the setup of capacitive deionization (CDI), where an effluent water stream is desalinated via the formation of an electrical double-layer at two oppositely polarized carbon electrodes. Yet, CDI can only be effectively applied to low concentrated solutions due to the intrinsic limitation of the electrosorption mechanism. By replacing the conventional porous carbon with MoS2/CNT binder-free electrodes, deionization of sodium and chloride ions was achieved by ion intercalation instead of ion electrosorption. This enabled stable desalination performance over 25 cycles in various molar concentrations, with salt adsorption capacities of 10, 13, 18, and 25 mg g-1 in 5, 25, 100, and 500 mM NaCl aqueous solutions, respectively. This novel approach of faradaic deionization (FDI) paves the way towards a more energy-efficient desalination of brackish water and even sea water.