Every year, thousands of tons of gaseous mercury are released globally, prompting the World Health Organization (WHO) in 2020 to designate mercury as one of the top 10 chemicals posing severe health risks. Therefore, removal of Hg 0 from the environment is imperative. Our study introduces [Mo 3 S(S 2 ) 6 ] 2− � [Mo 3 S 13 ] 2− -functionalized layered double hydroxide nanoparticles, (LDH−Mo 3 S 13 ), as an excellent sorbent for gaseous Hg 0 . This material achieved a remarkable sorption capacity of ∼2.33 × 10 3 mg/g for gaseous elemental Hg 0 . Such an enormously high sorption capacity makes this material the lead non-platinum-based Hg 0 gas sorbent known to date. Although sulfides of the Mo 3 S(S 2 ) 6 species of LDH predominantly serve as active sites for capturing gaseous Hg, their integration is essential for the accessibility of gaseous Hg 0 to the individual reactive active site between the LDH lamella. A heterogeneous reaction between the Hg 0 vapor and the solid LDH−Mo 3 S 13 sorbent enables the oxidation of gaseous Hg 0 to Hg 2+ , and the reduction of the S 2 2− groups to 2S 2− yields redox-driven formation of the nanocrystalline HgS onto the solid sorbents. Density functional theory (DFT) calculations provide further insights into the interactions between Hg 0 and S, indicating adsorption energy ranging from −8 to −19 kJ/mol. Moreover, the overall reaction enthalpy was calculated as −4048 kJ/mol, suggesting the spontaneous formation of HgS. This investigation unveils an atomistic understanding of the redoxdriven interactions between Hg 0 vapor and Mo 3 S(S 2 ) 6 species as well as the remarkably high mercury sorption capacity of LDH− Mo 3 S 13 , highlighting the potential of metal sulfide-functionalized LDHs for the efficient immobilization of gaseous elemental mercury.