Silica-silver nanocomposites (Ag-SBA-15) are a novel class of multifunctional materials with potential applications as sorbents, catalysts, sensors, and disinfectants. In this work, an innovative yet simple and robust method of depositing silver nanoparticles on a mesoporous silica (SBA-15) was developed. The synthesized Ag-SBA-15 was found to achieve a complete capture of Hg0 at temperatures up to 200 °C. Silver nanoparticles on the SBA-15 were shown to be the critical active sites for the capture of Hg0 by the Ag-Hg0 amalgamation mechanism. An Hg0 capture capacity as high as 13.2 mg·g-1 was achieved by Ag(10)-SBA-15, which is much higher than that achievable by existing Ag-based sorbents and comparable with that achieved by commercial activated carbon. Even after exposure to more complex simulated flue gas flow for 1 h, the Ag(10)-SBA-15 could still achieve an Hg0 removal efficiency as high as 91.6% with a Hg0 capture capacity of 457.3 μg·g-1. More importantly, the spent sorbent could be effectively regenerated and reused without noticeable performance degradation over five cycles. The excellent Hg0 removal efficiency combined with a simple synthesis procedure, strong tolerance to complex flue gas environment, great thermal stability, and outstanding regeneration capability make the Ag-SBA-15 a promising sorbent for practical applications to Hg0 capture from coal-fired flue gases.