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The slow redox kinetics and shuttling behavior of the intermediate lithium polysulfides constrain the further development of lithium–sulfur (Li–S) electrochemistry. A yolk–shell In2S3@void@carbon hybrid engineered to host the sulfur for Li–S batteries is prepared by using a multi-layered assembly method. The In2S3/electrolyte interface acted as powerful adsorption and activation sites for soluble polysulfides, which is demonstrated using density functional theory (DFT) calculations. Moreover, the carbon shell provides redundancy for volume-changes during the cycles. The results indicate that yolk–shell In2S3@S@C hybrid cathode shows good reversibility and rate capability, which preserves 563.6 mA h g−1 after 500 cycles at 0.5 C, indicating the potential for developing high-performance battery systems. [ABSTRACT FROM AUTHOR]