graphite anodes) and the lowest electrochemical potential (-3.04 V versus the standard hydrogen electrode). [5] However, the application of Li-metal anodes in batteries still faces many challenges due to its low coulombic efficiency (CE), rapid capacity decay, poor cycle life, [6] and safety concerns [7] resulting from the uncontrollable growth of dendritic Li during cycling. [8] On the one hand, Li dendrites may pierce the fragile solid electrolyte interface (SEI) and even separators, resulting in internal short circuits, thermal runway, and even the explosion of the battery. [9] On the other hand, Li dendrites can easily fall off from the bulk Li, reducing the utilization of active Li and the CE. [10] Therefore, preventing the formation of Li dendrites is the crucial step to realize the practical application of Li-metal batteries (LMBs) with high energy density. [11] To alleviate the abovementioned problems related to the growth of Li dendrites, enormous efforts have been devoted to finding solutions. These solutions can be roughly divided into five categories: the modification of the SEI layer by the addition of additives, [12] introduction of various ex-situ artificial SEI protective layers, [13] construction of 3D structured Li anodes, [14] utilization of solid-state electrolytes, [15] and design of functional separators. [16] Among these strategies, coatings or interlayers of the separator, such as MOFs, [16a] Al 2 O 3 , [16b] MnCO 3 , [16c] VS 2 flakes, [16d] carbon materials, [2b] and nonporous gel electrolytes, [17] are facile and convenient ways to suppress the growth of Li dendrites. All these works have achieved good results. Herein, we introduced the positively charged layer (PCL) to polypropylene (PP) separator. PCL is composed of polymer sidechains with freely moving multication groups, can regulate the lithium-ion deposition behavior in sub-nano scales.During the deposition process of a commercial PP separator cell, Li ions will deposit to regions with higher current density and then inevitably form protuberant Li metal tips (LMTs) due to the inherent heterogeneity of Li metal. [18] Then, the electric field strength around the formed LMTs will be significantly enhanced based on Gauss's flux theorem. Consequently, more Li ions will preferentially deposit around the LMTs to form Li dendrites. [19] However, unlike the reported strategies in the literature, this study is based on the "dynamic tip-occupying electrostatic shield" (DTOES) effect for achieving uniform Lithium-metal batteries (LMBs) have long been considered the "holy grail" of next-generation energy storage systems due to the unique advantages of Li metal, such as having a high specific capacity and the lowest potential. Unfortunately, the practical application of LMBs is seriously hindered by the uncontrollable growth of dendritic Li. To address this issue, a positively charged layer (PCL) with freely moving multication sidechains is successfully polymerized on a commercial polypropylene (PP) separator. The cationic groups on the ...