The performance of titanium dioxide (TiO2) for elemental mercury (Hg-0) removal was significantly increased when silver cooperates. Periodic density functional theory calculation demonstrated that the adsorption of Hg-0 over silver-deposited TiO2 composites were relative stronger than those in both isolated silver cluster and bare TiO2 by promoting electron transferred from Hg-0 to the deposited silver cluster and the entire TiO2. Furthermore, the formation of stable silver ions at the TiO2 interface acted as attractive sites for Hg-0 capture. The physical and chemical characterization demonstrated that the adsorption process start with Hg-0 deposits on a junction interface of silver ions and subsequently spillovers to form stable silver amalgam. Importantly, synergy between the deposited silver and TiO2 support represents an approach for Hg-0 attraction and retention, therefore, can be used for other hazardous materials mitigation. (C) 2018 Elsevier B.V. All rights reserved.