remarkable evolutions with continuous performance improvements, [4] after three decades of continuous research and development, the typical LIBs employ graphite (theoretical capacity of 372 mAh g −1) as the anode. [5] The energy density of LIB progressively approaches its theoretical limit. Therefore, exploring the next generation anode materials, which can break the ceiling of theoretical capacity of LIBs, is essential for the emerging applications to achieve wireless and green world. [6] Li metal is highly recognized as the very promising alternative anode material due to its low electrochemical potential of −3.04 V versus the standard hydrogen electrode and ultrahigh theoretical capacity of 3860 mAh g −1 , [7] which is almost 10 times of commercial graphite anode. Nevertheless, the disordered Li dendrite deposition during charge/discharge process motivates the dramatical fluctuation of the surface of Li anode, thus resulting in the break/ repair of the solid-electrolyte interphase (SEI) with severe phase migrations, electrolyte consumptions and thermal accumulations. [8] The unexpected microstructural Li dendrite can easily loss the electric connection with the bulk Li or current collector and subsequently form "dead Li," causing severe capacity loss. [9] Moreover, Li dendrite deposition not only aggravates battery performance with low Coulombic efficiency (CE) and rapid capacity decay, [10] but also engenders thermal runaway and even serious safety hazards caused by the internal shorting. [11] Therefore, preventing the lithium dendrite growth plays the key role to accomplish the next-generation highenergy-density and safe Li metal batteries (LMBs). [12] How to suppress the Li dendrite growth raises an inescapable question: why Li tends to deposit dendritic morphology? The formation of Li dendrite undergoes two process including Li nucleation and Li growth. [13] The growth process immediately follows nucleation and develops on the surface of nuclei with their incorporation into the structure of the Li metal lattice. Herein the final deposition morphology tightly relies on the Li nucleation and early growth. [14] Figuring out the Li nucleation and early growth is critical to further explore the dendrite inhibition strategies for safe and long-lifespan LMBs. Recently, many insightful and influential models have been proposed to understand the process of Li deposition from nucleation to early growth. [15] Specifically, 1) heterogeneous model describes the heterogeneous nucleation and early growth behavior; 2) surface diffusion model demonstrates Lithium (Li) metal is one of the most promising alternative anode materials of next-generation high-energy-density batteries demanded for advanced energy storage in the coming fourth industrial revolution. Nevertheless, disordered Li deposition easily causes short lifespan and safety concerns and thus severely hinders the practical applications of Li metal batteries. Tremendous efforts are devoted to understanding the mechanism for Li deposition, while the final depositio...