as supercapacitors and batteries, with high power/energy densities, are expected to play essential roles in our daily life as the dominant power sources for portable consumer electronics (e.g., smartphones, tablets, notebook PCs and camcorders), hybrid electric/plug-in-hybrid vehicles and smart grids. [1][2][3][4][5][6] The recently increased research efforts on 2D materials, i.e., graphene and its analogues, is to a great extent the result of the promise that they hold for technological applications including electronic devices, sensors, catalysts, energy conversion and storage devices, etc., by taking full advantage of their outstanding electrical, optical, chemical, and thermal properties. [7][8][9][10][11][12][13][14] Beyond graphene, other layered materials possessing various elemental compositions and different crystallographic structures, offer a broad portfolio of material's solutions with tunable chemical and physical properties for application as high-performance active components, which can operate as electrode materials for high-performance electrochemical energy storage devices. [4,15,16] Although graphene-based nanomaterials have demonstrated outstanding performance as electrodes in energy storage devices, new alternative nanomaterials should also be developed in order to further improve the electrochemical performance. Other 2D materials as graphene analogues (GAs) are expected to have broad implications in next generation of clean, efficient, and renewable energy systems. Layered materials of GAs refer to layered materials having similar structure as graphene, with planar topology and ultrathin thickness (single to few atomic layers). Typical GAs for energy storage include transition metal dichalcogenides (TMDs), transition metal oxides (TMOs)/ hydroxides (TMHs), metal sulfides, phosphorenes, MXenes, silicences, etc. (Figure 1). [17] Due to their thickness on the atomic scale, their inherent properties differ from those of their bulk lamellar systems. In particular, the quantum confinement of electrons in the 2D plane imparts them with unprecedented electrical and electronic characteristics ( Table 1). [18][19][20][21][22][23][24][25][26] Moreover, it is well known that the delivered specific capacity of electrode materials is closely related with the reaction kinetics during the charging/discharging process. [3] In view of their high surfaceto-volume ratio, GAs offer high specific surface areas (Table 1) to enable full utilization of all available sites of active electrode materials. [27][28][29][30] As a result, the exposed contact area is significantly enhanced between the electrodes and electrolytes, and also the paths for transport of charges are largely shortened.Energy crisis is one of the most urgent and critical issues in our modern society. Currently, there is an increasing demand for efficient, low-cost, lightweight, flexible and environmentally benign, small-, medium-, and large-scale energy storage devices, which can be used to power smart grids, portable electronic devices, and elect...