Lithium metal batteries (LMBs) are rechargeable battery systems that use a lithium metal anode along with intercalation or conversion-type cathodes. The high specific capacity and low electrochemical potential of lithium metal make LMBs a promising solution for thinner and lighter energy-storage systems. However, the widespread use of lithium metal anodes is hindered by issues such as uneven dendritic deposition and fragile solid electrolyte interface (SEI) formation. To address these challenges, this study explores the use of graphene as a substrate to stabilize lithium deposition. Specifically, two different graphene assemblies, layered and crumpled, are successfully fabricated on a copper current collector using an air-controlled electrospray process. Electrochemical tests demonstrate that both graphene structures effectively stabilize lithium deposition. Especially, the crumpled graphene structure maintains 98.3% Coulombic efficiency (CE) for 300 cycles in a half-cell configuration with a carbonate electrolyte. Furthermore, coupling the lithiated graphene anode with an NMC811 cathode in a full-cell battery under low negative/positive capacity ratio conditions results in improved anode stability over longer cycles.