Multiscale Simulation Drives the Rational Design of Lithium‐Sulfur Batteries

Abstract Computational methods have become a cornerstone for elucidating the nature of catalytic activity and electrocatalytic mechanisms in lithium‐sulfur (Li‐S) batteries. However, key factors such as the morphology, interfacial structure, and active sites of catalytic materials in Li‐S batteries are highly complex, making it difficult to fully interpret their mechanisms based solely on single‐scale simulations. Thus, achieving a multiscale understanding—spanning from the atomic‐scale to data‐driven approaches—has emerged as a critical yet challenging frontier in the design of Li‐S battery materials. This review adopts a multiscale simulation perspective to gain deeper insights into the structure–activity relationships within Li‐S battery catalysis. The paper begins by outlining recent advances and existing challenges in Li‐S batteries, followed by a systematic survey of research methodologies across four scales: electronic/atomic, molecular/interfacial, macroscopic, and data‐driven. Finally, this review summarizes the crucial role of multiscale computational simulations in advancing the understanding of various processes, including the design of cathode catalytic materials, simulations of electrode–electrolyte interfaces, mechanistic revelations of reaction conversion processes, and suppression of lithium dendrite formation at the anode. This review aims to offer methodological support for the development of high‐performance Li‐S batteries.