The separator is a crucial component in lithium batteries, as it physically separates the cathode and the anode while allowing ion transfer through the internal channel. The pore structure of the separator significantly influences the performance of lithium batteries, particularly lithium metal batteries. In this study, we investigate the use of a Janus separator composed of poly(ethylene terephthalate) (PET)−polytetrafluoroethylene (PTFE) fibers in lithium metal batteries. This paper presents a comprehensive analysis of the impact of this asymmetric material on the cycling performance of the battery alongside an investigation into the influence of two different substrates on lithiumion deposition behavior. The research findings indicate that when the rigid PET side faces the lithium metal anode and the soft PTFE side faces the cathode, it significantly extends the cycling lifespan of lithium metal batteries, with an impressive 82.6% capacity retention over 2000 cycles. Furthermore, this study demonstrates the versatility of this separator type in lithium metal batteries by assembling the lithium metal electrode with high cathode-loading capacities (4 mA h/ cm 2 ). In conclusion, the results suggest that the design of asymmetric separators can serve as an effective engineering strategy with substantial potential for enhancing the lifespan of lithium metal batteries.