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Abstract A stable lean‐electrolyte operating lithium–sulfur (Li–S) battery based on a cathode of Li₂S in situ electrocatalytically deposited from L₂S₈catholyte onto a support of metallic molybdenum disulfide (1T‐MoS₂) on carbon cloth (CC) is created. The 1T‐MoS₂significantly accelerates the conversion Li₂S₈catholyte to Li₂S, chemically adsorbs lithium polysulfide (LiPSs) from solution, and suppresses crossover of the LiPSs to the anode. These experimental findings are explained by density functional theory calculations that show that 1T‐MoS₂gives rise to strong adsorption of polysulfides on its surface and is electrocatalytic for the targeted reversible Li–S conversion reactions. The CC/1T‐MoS₂electrode in a Li–S battery delivers an initial capacity of 1238 mAh g⁻¹, with a low capacity fade of only 0.051% per cycle over 500 cycles at 0.5C. Even at a high sulfur loading (4.4 mg cm⁻²) and low electrolyte/S (E/S) ratio of 3.7 µL mg⁻¹, the battery achieves an initial reversible capacity of 1176 mA h g⁻¹at 0.5C, with 87% capacity retention after 160 cycles. The post 500 cycles Li metal opposing 1T‐MoS₂is substantially smoother than the Li opposing CC, with XPS supporting the role of 1T‐MoS₂in inhibiting LiPSs crossover.