In this research, an integrated dynamic and steady state (IDSS) method was developed to accelerate the discovery of new materials for the capture of Hg-0, a pollutant that is associated with fossil fuel utilization and has significant impacts on health and the ecosystem. A suite of metal sulfides and MoS2-based binary metal sulfides were evaluated using this method. It was found that the existence of MoS2 nanosheets promoted the Hg-0 removal efficiency of these metal sulfides. Among the MoS2-based metal sulfides studied in this research, Co-Mo-S and Cu-Mo-S exhibited excellent performance with an almost complete removal of Hg-0 at low temperatures. The results are superior to their corresponding metal oxides and the MoS2-containing adsorbent and are comparable to that of the commercial carbon-based adsorbent. Moreover, the working temperature windows for Hg-0 capture were found to be broader for the Mo-based binary metal sulfides than the corresponding metal oxides. The Co-Mo-S and Cu-Mo-S also showed better performance on He capture than other samples. It is proved that the IDSS approach is an effective and efficient method for the rapid screening of adsorbents for Hg-0 capture, which could be applied in the development of adsorption materials for environmental applications.