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Lithium‐sulfur (Li‐S) batteries hold immense promise as next‐generation energy storage due to their high theoretical energy density (2600 Wh kg⁻¹), low cost, and non‐toxic nature. However, practical implementation faces challenges, primarily from Li polysulfide (LiPS) shuttling within the cathode and Li dendrite growth at the anode. Optimized electrodes/electrolytes design effectively confines LiPS to the cathode, boosting cycling performance in coin cells to up to hundreds of cycles. Scaling up to larger pouch cells presents new obstacles, requiring further research for long‐term stability. A 1.45 Ah pouch cell, with optimized sulfur loading and electrolyte/sulfur ratio is developed, which delivers an energy density of 151 Wh kg⁻¹with 70% capacity retention up to 100 cycles. Targeting higher energy density (180 Wh kg⁻¹), the developed 1Ah pouch cell exhibits 68% capacity retention after 50 cycles. Morphological analysis reveals that pouch cell failure is primarily from Li metal powdering and resulting polarization, rather than LiPS shuttling. This occurs for continuous Li ion stripping/plating during cycling, leading to dendrite growth and formation of non‐reactive Li powder, especially under high currents. These issues increase ion diffusion resistance and reduce coulombic efficiency over time. Therefore, the study highlights the importance of a protected Li metal anode for achieving high‐energy‐dense batteries.

Prussian blue analogues (PBAs) cathodes can host diverse monovalent and multivalent metal ions due to their tunable structure. However, their electrochemical performance suffers from poor cycle life associated with chemo‐mechanical instabilities. This study investigates the driving forces behind chemo‐mechanical instabilities in Ni‐ and Mn‐based PBAs cathodes for K‐ion batteries by combining electrochemical analysis, digital image correlation, and spectroscopy techniques. Capacity retention in Ni‐based PBA is 96% whereas it is 91.5% for Mn‐based PBA after 100 cycles at C/5 rate. During charge, the potassium nickel hexacyanoferrate (KNHCF) electrode experiences a positive strain generation whereas the potassium manganese hexacyanoferrate (KMHCF) electrode undergoes initially positive strain generation followed by a reduction in strains at a higher state of charge. Overall, both cathodes undergo similar reversible electrochemical strains in each charge–discharge cycle. There is ~0.80% irreversible strain generation in both cathodes after 5 cycles. XPS studies indicated richer organic layer compounds in the cathode‐electrolyte interface (CEI) layer formed on KMHCF cathodes compared to the KNHCF ones. Faster capacity fades in Mn‐based PBA, compared to Ni‐based ones, is attributed to the formation of richer organic compounds in CEI layers, rather than mechanical deformations. Understanding the driving forces behind instabilities provides a guideline to develop material‐based strategies for better electrochemical performance.