namely natural graphite (NG) and artificial graphite. NG originates from organics rich in carbon under long-term hightemperature and high-pressure geological environments, while artificial graphite is obtained by artificial carbonization and graphitization of organics under high temperature. The main types of NG include flake graphite (FG) and microcrystalline graphite (MG). NG, such as flake FG, delivers high capacity owing to its larger anisotropic crystalline domains, while the artificial graphite with higher purity and larger fraction of edge planes caused by smaller crystalline size presents excellent electrochemical kinetics, long cycle life, but low initial Coulombic efficiency (ICE). [9,10] NG has drawn great attention as anode material in LIBs due to the outstanding features such as high energy density, excellent processability, and low cost. [11,12] By 2020, NG accounted for 39% of the anode material market compared with 58% of artificial graphite. [13] It should be noted that the market share of NG will continue to grow due to the requirements for reducing CO 2 emission and environmental footprint since the production of artificial graphite is energy-intensive, high cost, and time consuming. [14] China is rich in resources of NG and is the world's largest exporter of NG. [15] FG shows a typical layered and anisotropic structure in which large graphite crystals stack together within orientation. [16] When used as an anode material, FG presents high specific capacity and ICE, but poor cyclic stability due to the structure destruction caused by volume expansion. [17,18] MG presents isotropic structure, consisting of graphitic microcrystals randomly stacked together. The MG anode presents better cyclic stability and outstanding rate performance due to the small volume expansion and shortened lithium ion (Li + ) diffusion distance, but low ICE owing to the large surface area. [16] It should be noted that our group invented NG-based materials as early as 1992, [19][20][21] and introduced such low-cost materials in many aspects of applications, and finally into LIBs as commercial anodes in 1997. [22][23][24] To improve its electrochemical performance, surface modification such as carbon coating is essential for NG to form a stable solid electrolyte interface (SEI) layer, which can reduce the initial irreversible capacity, enhance the cyclability, and improve the low-temperature as well as thermal stability. [25] Besides, the NG can be hybridized with other carbon materials, including carbon nanotube (CNT), [26][27][28] Graphite, commonly including artificial graphite and natural graphite (NG), possesses a relatively high theoretical capacity of 372 mA h g -1 and appropriate lithiation/de-lithiation potential, and has been extensively used as the anode of lithium-ion batteries (LIBs). With the requirements of reducing CO 2 emission to achieve carbon neutral, the market share of NG anode will continue to grow due to its excellent processability and low production energy consumption. NG, which is abundant in Chi...