Recent reviews on LBs have provided a good overview of the developments of high energy density LBs based on diverse battery chemistries. [3][4][5][6] It is believed that the energy density of current LBs can be improved up to 300-350 Wh kg −1 in a short time by using high-nickel (Ni) content cathodes, silicon (Si) dominant anodes, and higher voltage electrolytes, but further progress is needed to achieve an acceptable lifetime for practical application. [7] In regards to long term goals, continued research and development (R&D) of next-generation LBs is necessary to meet the Battery500 Project target of a cell-level specific energy of 500 Wh kg −1 , [8] which necessitates a combination of both innovative battery chemistries (such as lithium (Li)-sulfur (S), Li-O 2 , Li-CO 2 , and so on), and cell configurations (improved active material ratio and cell integration). [9] However, the majority of current research efforts are dedicated to the R&D of battery materials while battery configurational design is relatively overlooked. Interestingly, with the progress in the development of water-in-salt electrolyte and the corresponding battery chemistry, aqueous LIBs are also possible to meet the Battery 500 Project target. A representative work is the aqueous LIBs that has been recently reported by Yang et al. which achieves a stable operation potential of 4.2 V and energy density of 460 Wh kg −1 . [10] It is great progress but worthy noting that the energy density calculation is based on the mass of anode and cathode. When the mass of the electrolyte is included, the full-cell energy density is dropped to 304 Wh kg −1 , revealing the important role of battery configurational design.Structural engineering provides a feasible and universal way to further improve the energy density of LBs without changing the fundamental battery chemistries. Since the battery's energy only comes from the electrically active materials in the electrodes, the core principle for the novel structural design of batteries is to minimize the ratio of inactive components while maintaining or improving battery performance per mass or volume of active material. Common strategies include the optimization of battery packaging with thinner, more robust materials, the reduction of electrode porosity with a higher packing density and increased electrolyte uptake, and the utilization of thick electrodes. The first is relatively hard to improve in a short time and would require a breakthrough in battery packaging materials with carefully evaluated cost and safety parameters. As for the reduction of electrolyte, it is also difficult toThe ever-growing portable electronics and electric vehicle markets heavily influence the technological revolution of lithium batteries (LBs) toward higher energy densities for longer standby times or driving range. Thick electrode designs can substantially improve the electrode active material loading by minimizing the inactive component ratio at the device level, providing a great platform for enhancing the overall energy densi...