Transition metal oxides (TMOs) have attracted considerable attention owing to their strong anchoring ability and natural abundance. However, their single‐site adsorption toward sulfur (S) species significantly lowers the possibility of S species reacting with Li+ in the electrolyte and increases the reaction barrier. This study investigates molecular modification by coupling the TMO structure with Li+ conductive polymer ligands, and vanadyl ethylene glycolate (VEG) is successfully synthesized by introducing organic ligands into the VOx crystal structure. In addition to the strong interaction between the VOx and lithium polysulfides via the V–S bond, the groups in the VEG polymer ligands can reversibly couple/decouple with Li+ in the electrolyte. Such dual‐site adsorption enables a smooth dynamic adsorption‐diffusion process. Accordingly, the VEG‐based Li–S cells exhibit excellent rate reversibility, cyclic stability, and a long cycle life without the addition of conducting agents. Encouragingly, the VEG‐based cells also exhibit close and excellent capacity decays of 0.081%, 0.078%, and 0.095% at 0, 25, and 50 °C (1 C for 200 cycles), respectively. This work provides a novel approach for developing advanced catalysts that can realize Li–S batteries with long‐term durability, fast charge‐discharge properties, and applications in a wide temperature range.

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