3860 mAh g −1 ), low redox potential (−3.04 V vs standard hydrogen electrode) and high capability to be coupled with high-voltage and/or high-capacity cathode materials. [1] However, the practical application of Li as an anode in rechargeable lithium batteries is still hindered by the uncontrollable growth of Li dendrites, low Coulombic efficiency (CE), and limited cycle life. [2] Numerous efforts have been made to address these issues. One of the strategies focuses on the design of suitable electrolytes by optimizing the concentration, [3] adding additives and fillers, [4] engineering highmodulus solid electrolytes and polymer electrolytes. [5] These advanced electrolytes are expected to have excellent electrochemical stability on the Li electrode and higher Young's modulus to resist the dendrite growth. [6] Further, developing stable host materials and nanostructured scaffolds to accommodate Li during the plating process has been employed to address the issues of large volume changes during lithium plating/stripping. [7] Recently, developing an artificial interfacial layer between the electrolyte and Li metal electrode has attracted tremendous attention in lithium metal batteries (LMBs). The interfacial layer can prevent side reactions, enable fast Li-ion diffusion, and suppress the Li dendrite growth for the efficient operation of Li metal anode. The side reactions and interfacial instability of Li metal lead to significant consumption of electrolyte. As a result, the resistance of the Li metal cell increases that leads to overpotential and ultimately short cell lifespan. Previous studies showed that various ceramics such as SiO 2 , TiO 2 , SnO 2 , and Al 2 O 3 are very promising interfacial layers to buffer the volumetric expansion of the anode. [8] Such ceramic layers are able to conduct Li + and block electron transport. [9] Lithiated multiwall carbon nanotubes and multilayered graphene with high mechanical rigidity have been reported as a controlled Li diffusion interface. [10] In addition, glass fibers, silica sandwiched between two separators, and silica@poly(methyl methacrylate) (SiO 2 @PMMA) nanosphere-modified Cu electrode has also been studied. [7c,11] These artificial layers improve wettability toward electrolyte, reduce the concentration of Li ions, and react with growing Li to suppress the dendrites. Organic/inorganic Lithium metal anodes are expected to drive practical applications that require high energy-density storage. However, the direct use of metallic lithium causes safety concerns, low rate capabilities, and poor cycling performance due to unstable solid electrolyte interphase (SEI) and undesired lithium dendrite growth. To address these issues, a radio frequency sputtered graphite-SiO 2 ultrathin bilayer on a Li metal chips is demonstrated, for the first time, as an effective SEI layer. This leads to a dendrite free uniform Li deposition to achieve a stable voltage profile and outstanding long hours plating/stripping compared to the bare Li. Compared to a bare Li anode, the graph...