Defective materials have been demonstrated to possess adsorptive and catalytic properties in lithium–sulfur (Li–S) batteries, which can effectively solve the problems of lithium polysulfides (LiPSs) shuttle and sluggish conversion kinetics during charging and discharging of Li–S batteries. However, there is still a lack of research on the quantitative relationship between the defect concentration and the adsorptive‐catalytic performance of the electrode. In this work, perovskites Sr0.9Ti1−xMnxO3−δ (STMnx) (x = 0.1–0.3) with different oxygen‐vacancy concentrations are quantitatively regulated as research models. Through a series of tests of the adsorptive property and electrochemical performance, a quantitative relationship between oxygen‐vacancy concentration and adsorptive‐catalytic properties is established. Furthermore, the catalytic mechanism of oxygen vacancies in Li–S batteries is investigated using density functional theory calculations and in situ experiments. The increased oxygen vacancies can effectively increase the binding energy between perovskite and LiPSs, reduce the energy barrier of LiPSs decomposition reaction, and promote LiPSs conversion reaction kinetics. Therefore, the perovskite STMn0.3 with high oxygen‐vacancy concentrations exhibits excellent LiPSs adsorptive and catalytic properties, realizing high‐efficiency Li–S batteries. This work is helpful to realize the application of the quantitative regulation strategy of defect engineering in Li–S batteries.

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The electrocatalytic conversion of polysulfides is crucial to lithium−sulfur batteries and mainly occurs at triple-phase interfaces (TPIs). However, the poor electrical conductivity of conventional transition metal oxides results in limited TPIs and inferior electrocatalytic performance. Herein, a TPI engineering approach comprising superior electrically conductive layered double perovskite PrBaCo 2 O 5+δ (PBCO) is proposed as an electrocatalyst to boost the conversion of polysulfides. PBCO has superior electrical conductivity and enriched oxygen vacancies, effectively expanding the TPI to its entire surface. DFT calculation and in situ Raman spectroscopy manifest the electrocatalytic effect of PBCO, proving the critical role of enhanced electrical conductivity of this electrocatalyst. PBCO-based Li−S batteries exhibit an impressive reversible capacity of 612 mAh g −1 after 500 cycles at 1.0 C with a capacity fading rate of 0.067% per cycle. This work reveals the mechanism of the enriched TPI approach and provides novel insight into designing new catalysts for high-performance Li−S batteries.

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