fabricated. Combined with controlled synthesis, MOF materials are endowed with abundant various of structures, morphologies, and properties. [8-11] In addition, the as-prepared MOFs can be artificially modified via postsynthetic approaches utilizing their available pores and active sites of metal clusters or linkers. [12,13] As a result, not only the number of MOFs is further increased but also many interesting properties, such as high specific surface areas, tailorable pore sizes, modifiable structures, and properties are endowed with MOFs, which make them become potential candidates in storage/separation, catalysis, sensing, etc. [14,15] Another important application of MOFs is that they can act as conductive materials for electrocatalysis, sensing, and energy conversion, etc. [16-19] The existence of quantitative amounts of active metal centers, permanent porosity, and structural rigidity can facilitate surface contact and mass transfer as well as increase catalysis stability, making MOFs as ideal electrocatalysts. [20-22] In addition, they possess high specific surface areas, tunable bandgaps, and good charge transport properties, which extend their applications in sensing and energy storage. [23] Besides, the morphologies and characteristics of MOFs can be artificially modified to form 1D, 2D, or 3D structures via liquid phase selfassembly, physical/chemical exfoliation, layer-by-layer assembly, etc., promoting their applications in electrochemical devices and electronics. [24-26] With further structural design through postsynthesized modification, the performances of MOFs can be largely improved, facilitating their applications as conductive materials. [27-29] However, most MOFs are intrinsically electrically insulated, which seriously hinders their electrochemical applications. [29] The connected rigid metal ions and redox-inactive organic ligands increase the energy barrier for electron transfer, making them as electrical insulators. To overcome the drawbacks of MOFs, many feasible strategies have been adopted to promote the electron transfer in the structures of MOFs. [27,30-32] The high electrical conductivity of MOFs can be realized by integrating the conjugated planes or 1D chains in the structures, which relies on particular structural designs. [33-37] The conductivity of the MOFs can also be increased via doping with guest Metal-organic frameworks (MOFs) have aroused worldwide interest over the last two decades due to their various excellent properties, such as porosity, modifiability, stability, etc. Based on these unique features, they have been widely exploited for applications from electrocatalysis to electrochemical devices. However, most MOFs are inherently insulated due to the lack of free charge carriers and low-energy barriers for charge transfer, which largely restricts their further electrochemical applications. By imparting MOFs with electrical conductivity, their electrochemical process and catalysis efficiency can be effectively improved. Similarly, their applications in sensors, secon...