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The commercialization of lithium–sulfur batteries with ultra‐high theoretical energy density is restricted mainly by the notorious polysulfides “shuttle effect” and slow Li2S redox reaction kinetics. A sulfur host material with high catalytic activity and high conductivity is greatly desired to improve its electrochemical performance. Herein, a sulfur host material, etched cotton@petroleum asphalt carbon (eCPAC), with high specific surface area and excellent catalytic activity, is demonstrated based on a synergistic strategy of introducing intrinsic lattice defects and composite carbon structure. Benefiting from in situ coupling of amorphous and crystalline materials, eCPAC exhibits high conductivity and high sulfur adsorbability. Furthermore, eCPAC containing dual intrinsic defect sites can catalyze the bidirectional sulfur chemistry of Li2S and capture polysulfides, which is also demonstrated by systematic density functional theory calculations and the potential intermittent titration technique. S@eCPAC/Li cells exhibit excellent cycling stability and rate performance, with an average capacity decay rate of only 0.05% over 1000 cycles at 0.5 C and even 0.03% over 600 cycles at 5 C. Meanwhile, the practicality of eCPAC is proven in high‐load batteries and pouch batteries. eCPAC provides a reliable strategy for achieving a win–win situation of capturing polysulfides and accelerating Li2S redox kinetics.

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Achieving stable cycling of high‐voltage solid‐state lithium metal batteries is crucial for next‐generation rechargeable batteries with high energy density and high safety. However, the complicated interface problems in both cathode/anode electrodes preclude their practical applications hitherto. Herein, to simultaneously solve such interfacial limitations and obtain sufficient Li+ conductivity in the electrolyte, an ultrathin and adjustable interface is developed at the cathode side through a convenient surface in situ polymerization (SIP), achieving a durable high‐voltage tolerance and Li‐dendrite inhibition. The integrated interfacial engineering fabricates a homogeneous solid electrolyte with optimized interfacial interactions that contributes to tame the interfacial compatibility between LiNixCoyMnzO2 and polymeric electrolyte accompanied by anticorrosion of aluminum current collector. Further, the SIP enables a uniform adjustment of solid electrolyte composition by dissolving additives such as Na+ and K+ salts, which presents prominent cyclability in symmetric Li cells (>300 cycles at 5 mA cm−2). The assembled LiNi0.8Co0.1Mn0.1O2 (4.3 V)||Li batteries show excellent cycle life with high Coulombic efficiencies (>99%). This SIP strategy is also investigated and verified in sodium metal batteries. It opens a new frontier for solid electrolytes toward high‐voltage and high‐energy metal battery technologies.