of Li-S technology is still impeded by intrinsic material challenges. First, sulfur and its discharge product lithium sulfide are insulating in nature, which deteriorates the active-material utilization and leads to sluggish redox-reaction kinetics. [2] Second, during charge and discharge, polysulfide intermediates (Li 2 S x , 4 ≤ x ≤ 8) form and easily dissolve into the liquid electrolyte. The dissolved polysulfides tend to migrate from the cathode to the anode side, causing unwanted parasitic reactions with lithium-metal anode and active-material loss from the sulfur cathode. These drawbacks lead to an irreversible capacity fade and low Coulombic efficiency. [3] Additionally, the degradation of anode and volume changes of sulfur species during reaction also undermine the electrochemical stability and cycle life of Li-S batteries, challenging the practical use of Li-S technology. [4,5] Intensive studies have been devoted to addressing the aforementioned problems, including new cathode design, [6][7][8][9] functional interlayer/separator fabrication, [10][11][12] efficient anode protection, [13][14][15][16] and optimized electrolyte formulas. [17][18][19][20] In view of cathode modification, it has been demonstrated that nonpolar carbon matrix with only physical polysulfide confinement may not be enough for high-loading cell performance during long cycle life. [21][22][23] Thus, numerous efforts have been focused on the chemical restriction for polysulfides to further improve the electrochemical functionality. [4,23] Transition-metal compounds, including metal oxides, [24] sulfides, [21] nitrides, [25] and carbides, [26] have been proven as efficient polysulfide traps by offering chemical polysulfide-adsorption sites. Among them, metal sulfides attract particular interest due to their strong sulfiphilicity together with multiple thermodynamically stable crystal structures and stoichiometric compositions. [27] For instance, cobalt disulfide (CoS 2 ), [21] titanium disulfide (TiS 2 ), [28,29] and iron disulfide (FeS 2 ) [30] have been applied as sulfur hosts and have been demonstrated with a strong chemical interaction capability toward migrating polysulfides. [23] However, these metal sulfides mainly exist in the form of large particles with varying levels of agglomeration, greatly shrinking the surface area for polysulfide adsorption and limiting the amount of sulfur species that could be loaded. [27] Accordingly, the sulfur cathodes used in most metal sulfide-related reports have an insignificant sulfur content of less than 60 wt% and a low sulfur A unique 3D hybrid sponge with chemically coupled nickel disulfide-reduced graphene oxide (NiS 2 -RGO) framework is rationally developed as an effective polysulfide reservoir through a biomolecule-assisted self-assembly synthesis. An optimized amount of NiS 2 (≈18 wt%) with porous nanoflower-like morphology is uniformly in situ grown on the RGO substrate, providing abundant active sites to adsorb and localize polysulfides. The improved polysulfide adsorptivity from sul...