Atomic‐Level Insight of Carbon‐Based Anodes for Advanced Sodium Storage: Electrochemical Mechanisms and Molecular Simulation‐Assisted Modification

Hard carbon (HC) has become one of the preferred anode materials for high‐performance sodium‐ion batteries (SIBs) due to its abundant reserves, unique structure, and high specific capacity. However, due to its complex microstructure, advances in the Na + storage mechanism and electrochemical behavior of HC remain limited, and most breakthrough reports are still confined to experimental synthesis. As an emerging computational tool based on quantum mechanics, density functional theory (DFT) has been widely used in computational materials science in recent years, greatly deepening the fundamental understanding of the internal electronic structure of materials. Therefore, this work reviews the Na + storage mechanism in various HC anode materials from the viewpoint of first‐principles simulations, aiming to clarify the composition‐performance correlation by combining theoretical analysis with experimental results. Secondly, this paper summarizes the DFT‐based evaluation and analytical tools for the sodium storage performance of HC anodes, and conducts targeted prediction and structural design of emerging carbon materials based on available experimental data. Finally, the future development prospects of HC materials in theoretical computation are outlined.