Suppressing Universal Cathode Crossover in High-Energy Lithium Metal Batteries via a Versatile Interlayer Design**

The universal cathode crossover such as chemical and oxygen has been significantly overlooked in lithium metal batteries using high-energy cathodes which leads to severe capacity degradation and raises serious safety concerns. Herein, a versatile and thin (≈25 μm) interlayer composed of multifunctional active sites was developed to simultaneously regulate the Li deposition process and suppress the cathode crossover. The as-induced dual-gradient solid-electrolyte interphase combined with abundant lithiophilic sites enable stable Li stripping/plating process even under high current density of 10 mA cm⁻². Moreover, X-ray photoelectron spectroscopy and synchrotron X-ray experiments revealed that N-rich framework and CoZn dual active sites can effectively mitigate the undesired cathode crossover, hence significantly minimizing Li corrosion. Therefore, assembled lithium metal cells using various high-energy cathode materials including LiNi_0.7Mn_0.2Co_0.1O₂, Li_1.2Co_0.1Mn_0.55Ni_0.15O₂, and sulfur demonstrate significantly improved cycling stability with high cathode loading. © 2023 Wiley-VCH GmbH.