Significant efforts are being made to develop high-performance battery materials, particularly active materials. However, material-dependent strategies for increasing energy density face challenges such as raw material costs and supply limitations, reducing their versatility to some extent. In this regard, the development of efficient battery designs can be a universal approach to increasing the energy density of lithium-ion batteries with relatively low dependence on material properties. Herein, a novel configuration of an electrode-separator assembly is presented, where the electrode layer is directly coated on the separator, to realize lightweight lithium-ion batteries by removing heavy current collectors. Even on the hydrophobic separator, a poly(vinyl alcohol) binder enables uniform and scalable coating of aqueous electrode slurries through molecular interactions with the separator surface. Moreover, carbon nanotubes are utilized to reinforce the electronic conduction of the electrode, providing consistent electronic pathways regardless of SEI formation. Furthermore, owing to the superior permeability of liquid electrolytes through this electrode-separator assembly, a multilayered electrode-separator assembly can be suggested to further increase energy density when combined with a lithium metal anode. This lithium metal battery can achieve an areal capacity of ≈30 mAh cm−2 and an enhanced energy density of over 20% compared to conventional battery configurations.