Mercury (Hg) contamination in soil is a paramount concern to the environment and public health. Yet, effective in situ remediation technologies have been lacking. In this study, a novel thiol-functionalized graphene oxide/FeMn (SGO/Fe-Mn) composite was prepared and investigated for in situ immobilization of Hg in contaminated soil. Batch tests showed that application of SGO/Fe-Mn at doses of 0.4% and 0.8% effectively reduced H2O, H2SO4 and HNO3 , CH3 COOH, and CaCl2 -extractable Hg by 90.3-98.9% and 96.5-98.9%, respectively, upon equilibrium after 72 d. An increasing of soil moisture content from 0 to 12.5% significantly enhanced the immobilization efficiency from 75.0% to 97.6%. XRD, FTIR, and XPS analyses suggested that the composite mainly immobilized Hg through surface complexation and chemical precipitation. Sequential extraction procedure demonstrated that the composite promoted the conversion of more accessible Hg (exchangeable and carbonate fractions) into the less accessible forms, i.e., oxides, organic matter, and residual fractions, resulting in substantially reduced environmental risk of Hg. The application of SGO/Fe-Mn enhanced soil cation exchange capacity, available N and K, and total organic carbon, and can be used to effectively improve soil properties. Moreover, immobilized Hg in soil by this composite remained stable over one year. The present study demonstrates the potential and viability of SGO/Fe-Mn for enhanced immobilization of Hg in soil and sediment.