is still the most popular cathode material in the LIBs for 3C products, mainly owing to its extraordinarily high tap density, [2] since there is a stricter requirement on the volumetric energy density. To reduce the amount of high-cost Co, part of Co was substituted by Ni and Mn with the generation of Li(Ni x Co y Mn z )O 2 (NCM, x + y + z = 1), which not only improves the structural and thermal stability but also allows more reversible extraction-intercalation of Li + and so endows more capacity, making it currently the dominant cathode materials in the market of power batteries of EVs. [3] Currently, compared with internal combustion engine vehicles, the main concerns for the popularization of EVs are the higher price, lower continue voyage course, and heavier safety risk, mainly resulting from the LIBs.For NCM cathodes, the capacities increase gradually with the increment of Ni contents; for instance, from Li(Ni 0.5 Co 0.2 Mn 0.3 )O 2 (NCM523) to Li(Ni 0.8 Co 0.1 Mn 0.1 )O 2 (NCM811), the capacity rises from 165 to 200 mAh g −1 , around 20% promotion. [4] However, with the increment of capacity, more Li + will reversibly intercalate into and extract from the NCM layered structure, resulting in larger volumetric change, more intergranular microcracks, and heavier interfacial reactions. [5] In addition, with the increase of Ni content, more superficial Ni 4+ ions lead to heavier catalytic oxidation of electrolytes, causing more serious capacity fading and safety risks. [6] To reduce the intergranular microcracks