“…Two-dimensional (2D) materials that are exfoliated from their layered precursors have the merit of high surface area, good electronic conductivity, and faradaic charge storage capabilities, rendering them highly promising for ion adsorption applications. − Several 2D materials such as transition metal carbides (MXene), − transition metal dichalcogenides, − and graphitic carbon nitrides have been tested for capacitive deionization . However, the study is continuously ongoing to further improve the physical and electronic properties of 2D materials via numerous strategies such as doping, oxygen vacancy, and interface modulation. , Among these techniques, interface modulation can increase the electronic conductivity and the surface area. − Interface modulation via the electrostatic self-assembly of oppositely charged nanosheets has received particular interest in recent years due to the excellent coupling at the heterointerface, giving rise to outstanding electrochemical properties. − A range of self-assembled two-dimensional materials such as MnO 2 /graphene, Ti 0.87 O 2 /N-doped graphene, MoS 2 /graphene, and Ni–Co–Al LDH/MXene have displayed tremendous potential for energy storage and conversion applications . The ordered channels and interlayer galleries of 2D heterostructures could facilitate ion transport, increase ion accessible sites, and reduce the charge transfer resistance across the heterointerface .…”