Heterostructure materials integrating the unique physical and chemical properties of each heterogeneous component are highly promising for optimizing lithium-sulfur batteries. However, precisely regulating the interface microstructures of heterostructures at the atomic scale still lacks effective means, and the law of interface microstructures affecting the properties of heterostructures is not yet clearly understood. Herein, an atomic-scale regulation strategy is presented to construct heterostructure materials containing the high-energy Fe