CoMoS/γ-Al2O3 sorbent was prepared via incipient wetness impregnation (IWI) and sulfur-chemical vapor reaction (S-CVR) methods and tested in terms of its potential for Hg(0) capture. It was observed that the CoMoO/γ-Al2O3 showed a Hg(0) capture efficiency around 75% at a temperature between 175 and 325 °C while CoMoS/γ-Al2O3 achieved almost 100% Hg(0) removal efficiency at 50 °C. The high removal efficiency for CoMoS/γ-Al2O3 remained unchanged for 2000 min in the test. Its theoretical capacity for Hg(0) capture was found to be 18.95 mg/g based on the Elovich model. The ability of this material for Hg(0) capture is atributed to the MoS2 nanosheets coated on surface of the maro- and meso-pores of γ-Al2O3. These MoS2 are two-dimensional transition-metal dichalcogenide (2D TMDC) assembled with unsulfided cobalt atoms at the edges. It is believed that these MoS2 nanosheets provided dense active sites for Hg(0) capture. The removal of Hg(0) at low temperatures was achieved via the combination of Hg(0) with the chalcogen (S) atoms on the entire basal plane of the MoS2 nanosheets with coordinative unsaturated sites (CUS) to form a stable compound, HgS.