An attempt was made to recover Ag(I) using MoS2 nanosheets as adsorbent. The adsorption process was investigated through adsorption kinetics and isotherm tests, and the adsorption mechanism was revealed by XPS and DFT calculations. The results indicated that adsorption process was well consistent with Langmuir isotherm model. The high Ag(I) adsorption capacity of MoS2 (780 mg/g) could be attributed mainly to the complexation of Ag-S, along with insignificant complexation of Ag-O. The interaction between Ag(I) and MoS2 surface was in the form of orbital hybridization of Ag(I) with S and O.