In this study, we report for the first time a novel type of sorbent that can be used for mercury adsorption from the air-based off-gasses-vermiculite impregnated with alkali polysulfides and thiosulfates. In contrast to other sorbents, vermiculite exhibits superior thermal stability in air and low adsorption capacity for organic vapors. This allows for a more favorable design of the soil remediation unit-direct coupling of thermal desorber with catalytic oxidizer using air as a carrier gas. In the bench-scale test at 180 °C, the sulfur/vermiculite sorbent exhibited significantly higher efficiency for the adsorption of mercury vapor from the off-gasses than the commercial sulfur/activated carbon sorbent at its highest operating temperature (120 °C). The average mercury concentration in the adsorber off-gas decreased from 1.634 mg/m3 for the sulfur/activated carbon to 0.008 mg/m3 achieved with impregnated vermiculite. The total concentration of organic compounds in the soil after thermal desorption was below the detection limit of the employed analytical method.