The use of two mercury and arsenic removal media: A) a sulfur-impregnated organoclay; and B) a coupling agent-reacted organoclay, wherein the coupling agent preferably contains a mercapto, disulfide, tretrasulfide and/or polysulfide end group provides mercury removal media having increased reactivity, stability, and synergistic mercury removal ability. The preferred mercury removal media described herein is prepared by reacting an organophilic clay containing onium ions A) with elemental sulfur; and B) with a sulfur-containing coupling agent, preferably containing a mercapto, disulfide, tetrasulfide, and/or polysulfide moiety.