Lithium–sulfur batteries are nearly ready to be commercialized. However, each material composition has specific challenges regarding its adaption to state of the art production lines of lithium‐ion batteries. The influence of the dispersing and calendering process on the battery performance is investigated with an easy‐to‐implement material approach and a solvent‐based process. The slurry is treated by different dispersing intensities using an extruder and a triple roller mill, which leads to increased energy densities. The coating is calendered to increase the energy density by maintaining the specific capacity. The reactions within the sulfur cathodes are investigated by evaluating the potentials of the upper and lower voltage plateaus. It was determined that the variation of the process parameters leads to a changed reactivity of the polysulfide reactions but not to a shift of the sulfur utilization within the sulfur cathodes. The process parameters influence the pore structure of the cathode, resulting in different sensitivities for higher C‐rates.

Lithium–sulfur batteries (LSBs) that utilize sulfur and lithium (Li) metal as electrode materials are highly attractive for transportation applications due to their high theoretical gravimetric energy density. However, two major challenges currently impede the commercialization of LSB, which are the formation of Li dendrites and polysulfide shuttling. To mitigate these two effects, a protective film or artificial solid–electrolyte interface (SEI) can be applied directly to the Li‐metal surface. Herein, the preparation of freestanding polyethylene oxide (PEO)‐based films using tape casting as a scalable coating technique is presented. Moreover, the films are applied directly to the Li surface via a solvent‐free method. To demonstrate the suitability of the developed PEO‐based films, the long‐term cycling performance of the lithium–sulfur cells is discussed. It is shown that the cells with the Li‐metal surface protected by PEO‐based films achieve better stability and reproducibility, reaching ≈400 mA h g S−1 after 250 cycles compared to ≈200 mA h g S−1 after 250 cycles for the bare Li‐metal electrode. An extensive postmortem analysis of the Li‐metal electrode surface with scanning electron microscopy is additionally shown, revealing that the PEO‐based artificial SEIs form uniformly with a low level of defect layers at the interface with the Li‐metal electrode, which indicates the creation of a stable SEI.