extremely low electrode potential (−3.04 V versus standard hydrogen electrode), [1,2] it suffers terribly from an in-homogeneous Li deposition and a rough solid electrolyte interphase (SEI) being caused by continuous electrolyte reduction because its electrochemical potential lies above the lowest unoccupied molecular orbital (LUMO) of non-aqueous electrolytes. Hence, an uneven Li + flux prevails and is exceedingly dense at the tip/needle-like points to promote dendritic growth and concurrent deposition of "dead Li" reflected as low coulombic efficiency, capacity fade, and safety concerns in a battery. [3][4][5][6] Several attempts to realize the long-term stability of metal anodes through Li protection involving structured/patterned Li-metal anodes, [7] pre-formed artificial SEIs, [8,9] ex-situ surface protective layers, [10][11][12] electrolyte modification (redox mediators, high Li-salt concentration), [13][14][15] self-healing surfaces, [16,17] and cycling protocols [18,19] have been reported to suppress dendrite growth. Unfortunately, the developed artificial SEIs end up with features such as acute thickness, extraneous species, poor and incompatible electrode-electrolyte interface, and low interphase wettability, compromising the concentration of liquid electrolyte and Li content.Recently, it has been reported that the use of lithiophilic carbon-based materials would be an effective strategy to control and regulate nucleation sites with a lower polarization. [20][21][22] Several lithiophilic carbons such as carbon fibers, [23] porous carbon, [24,25] graphene matrix, [26,27] reduced graphene oxide (rGO), [28,29] and carbon nanotubes [30,31] have been widely engineered to establish a regulated Li redeposition with multiple battery components as protected Li metal, Li hosts, coated on the separator, and electrolyte additive. However, their cycle life remains uncertain due to the problems of top deposition that could again trigger dendrite or "dead Li" leading to surface roughness. [7][8][9][10][11][12][13][14] Worse, the reported carbons are mostly non-site and non-size specific, which collapses in a longterm cycling and additionally adds up to an inactive cell mass (0.4-3 mg cm −2 ) making the design and collective interpretation empirical. [23][24][25][26][27][28][29][30] Recently, the size-specific characteristics of graphene sheets unveiled as N,S-co-doped graphene, graphene Dendrite growth and in-homogeneous solid electrolyte interphase (SEI) buildup of Li metal anodes hinder the longtime discharge-charge cycling and safety in secondary metal batteries. Here, the authors report an in-situ restructured artificial lithium/electrolyte SEI exposing an ultrasmooth and thin layer mediated through graphene quantum dots (GQDs). The reformed artificial interphase comprises a mixture of organic/inorganic-rich compositions alike as mosaic interphase, albeit the synergistic effect mediated via hydroxylated GQDs involving redeposition-borne lithium, and its accumulated salts, facilitate a homogeneous and ultrasmooth n...