nanobelts), 2D materials exhibit exceptional physical properties including large theoretical surface area, tunable electronic properties, high optical transparency, and excellent mechanical properties. [2] However, the strong re-stacking tendency of 2D materials caused by van der Waals interaction may result in serious loss of surface area, which inevitably weakens their unique properties. Besides, 2D materials always show intrinsic deficiencies for specific applications, despite the merits mentioned above. As a typical example, TMDs possess high theoretical specific capacities for lithium-ion storage but exhibit unsatisfied cyclability and rate capability in practice, because of their aggregation, low conductivity as well as huge volume expansion during lithium-ion insertion/extraction. [3] One effective way to solve these problems is to construct hybrid nanostructures based on 2D materials. [4][5][6][7][8] Hybrid nanostructures, as a class of composite materials, are composed of two or more nanostructured building blocks. [9,10] Hybrid nanostructures not only can energetically combine the intriguing merits and overwhelm the deficiencies of each building block, but also may generate new functions and properties. [3][4][5][6][7][8][11][12][13] These advantages make hybrid nanostructures based on 2D materials highly promising for practical applications with high performance. [14][15][16][17][18] Regarding the multicomponent composition of hybrid nanostructures, the interfacial interaction between the building blocks lays the foundation for structural and morphological stability, thereby influencing the functions and properties of the resulting hybrid nanostructures. [19][20][21][22] In this sense, the rational design and construction of reliable interfacial interaction for hybrid nanostructures are not only important for achieving improved performance, but also critical for understanding the fundamentals of structureproperty relationship.Generally, there are five types of interfacial interactions, i.e., covalent bond, coordination bond, hydrogen bond, π-π interaction, and electrostatic interaction. [19][20][21][22] Covalent bond and coordination bond are much stronger than the other three in terms of bond energy, so the former two are more favorable for constructing hybrid nanostructures with reliable interfacial interaction. [19] However, most 2D materials are chemically inert, which means the covalent modification is not suitable for them. Alternatively, there are coordination atoms in most of 2D materials and their derivatives, and hence coordination 2D materials have received tremendous scientific and engineering interest due to their remarkable properties and broad-ranging applications such as energy storage and conversion, catalysis, biomedicine, electronics, and so forth. To further enhance their performance and endow them with new functions, 2D materials are proposed to hybridize with other nanostructured building blocks, resulting in hybrid nanostructures with various morphologies and structures. The prop...