Higher expectations are being placed on the environmental specifications and energy storage performance of advanced energy storage devices as a result of growing environmental concerns and the rapid advancement of modern technology [1,2]. Globally, photovoltaic and wind farms are being developed to meet the power and range needs of electric and hybrid vehicles, utilizing energy from intermittent sources. However, conventional lithium-ion batteries, with energy densities approaching their theoretical ceiling of approximately 250–300 Wh kg−1, fail to meet the range requirements of vehicles.

Lithium‑sulfur (LiS) batteries are one of the most promising candidates for next-generation battery systems due to their ultra-high theoretical performance. LiS batteries have a theoretical energy density of 2, 600 Wh kg−1 and a theoretical specific capacity of 1, 675 mAh g−1, while the cathode material element sulfur is naturally abundant, environmentally friendly, and available at a low cost. Due to these advantages, LiS batteries are one of the most promising candidates for next-generation energy storage [3,4]. However, LiS batteries still have some shortcomings that seriously hinder their practical application. First, the low conductivity of S (about 5 × 10−30 S cm−1 at room temperature) and the final reduction products (Li2S and Li2S2) are difficult to meet the requirements of the battery cathode [[5], [6], [7]]. Second, the volume expansion of sulfur species (∼80 %) after lithiation can destroy the structure of the S electrode in an unconstrained structure, leading to continuous shedding of the active material and reducing the Coulomb efficiency and stability of the LiS batteries [[8], [9], [10], [11]]. Thirdly, Polysulfides (Li₂Sₙ, 4 ≤ n ≤ 8) derived from active materials exhibit high solubility in conventional ether-based electrolytes. Driven by concentration gradients and electric field forces, these species shuttle between the cathode and anode through the separator, imposing three severe consequences: Parasitic reactions at the lithium anode cause active sulfur loss; Continuous redox cycling induces accelerated self-discharge (>5 %/day); Corrosive deposition on the anode forms insulating Li₂S/Li₂S₂ layers. This phenomenon ultimately triggers rapid capacity fading and reduces practical energy density by 30–50 % in LiS systems [[12], [13], [14], [15], [16]].In the past, as the mechanism of LiS batteries operation has been studied in depth, various methods have been developed to suppress the shuttle effect, which has greatly improved the electrochemical performance of LiS batteries [[17], [18], [19], [20], [21], [22]]. In the early studies, efforts were made to control the diffusion of lithium polysulfides using highly conductive, highly porous carbon materials. Carbon-based materials with different pore structures have been developed, including microporous carbon [[23], [24], [25], [26], [27], [28]], mesoporous carbon [[29], [30], [31], [32], [33]], and graded porous carbon [[34], [35], [36], [37], [38]], to load sulfur as the positive electrode. With the continuous in-depth research on the operation mechanism of LiS batteries, many new materials, such as metal compounds [[39], [40], [41]], alloys [[42], [43], [44]], and metal-organic frameworks (MOFs) [[45], [46], [47]], have been applied not only for the adsorption and catalysis of lithium polysulfides. Different site-specific modifications in lithium polysulfides to suppress the shuttle effect have also been made by reducing the solubility of electrolyte [[48], [49], [50], [51]], using solid electrolytes [[52], [53], [54]], and constructing artificial solid electrolyte interphase (SEI) membranes [53,55,56].There are many reviews about LiS batteries especially for suppressing shuttle effect of lithium polysulfides, but most of them focused on different host materials and separator modifications. For example, Li et al. reported the unique advantages of hollow micro- and nanostructures applied to the main body material of LiS batteries [57]. Pang et al. summarized the chemical interactions of lithium polysulfides based on the body material [58]. The progress of separator research in advanced LiS batteries is reviewed by Wei et al. [59] Deng et al. summarized various methods to limit the diffusion of lithium polysulfides at both cathode and separator sites based on the diffusion path of lithium polysulfides and discussed their mechanisms of action [60]. Liang et al. summarized recent advances in single atom catalysts (SACs) for lithium metal anodes, S cathodes, and separators and how SACs work [61]. These early reviews provide a comprehensive overview of LiS batteries mainly by classifying them according to the type of applied material or site of the battery but rarely highlight comprehensive strategies to suppress shuttle effects through interactions.Lithium polysulfides undergo complex chemical, electrochemical, and physical behavior during LiS battery operation. The shuttle effect and other problems can be solved by effectively changing the behavior of lithium polysulfides using appropriate material interactions on lithium polysulfides. Herein, based on directional quantification assessment, we focus on the affinity/repulsion interactions between materials at distinct constituent units of lithium‑sulfur batteries and polysulfides. We systematically analyze how these site-specific interactions with defined directionality and intensity can be leveraged to suppress polysulfide shuttle effects. This review aims to present a new perspective on the design strategies applied to LiS battery materials from the perspective of affinity/repulsion interactions in combination with the pathway of shuttle effect (Fig. 1). Questions and perspectives on future research of LiS batteries based on affinity/repulsion interactions are also presented.