Soils, especially permafrost in the Arctic and the Tibetan Plateau, are one of the largest reservoirs of mercury (Hg) in the global environment. The Hg concentration in the grassland soils over the Tibetan Plateau and its driving factors have been less studied. This study analyzes soil total mercury (STHg) concentrations and its vertical distribution in grassland soil samples collected from the Tibetan Plateau. We adopt a nested-grid high-resolution GEOS-Chem model to simulate atmospheric Hg deposition. The relationship between STHg and soil organic carbon (SOC), as well as atmospheric deposition, are explored. Our results show that the STHg concentrations in the Tibetan Plateau are 19.8 +/- 12.2 ng/g. The concentrations are higher in the south and lower in the north in the Tibetan Plateau, consistent with the previous results. Our model shows that the average deposition flux of Hg is 3.3 mu g m(-2) yr(-1), with 57% contributed by dry deposition of elemental mercury (Hg-0), followed by dry (19%) and wet (24%) deposition of divalent mercury. We calculate the Hg to carbon ratio (R-Hg:C) as 5.6 +/- 6.5 mu g Hg/g C, and the estimated STHg is 86.6 +/- 101.2 Gg in alpine grasslands in the Tibetan Plateau. We find a positive relationship between STHg and SOC in the Tibetan Plateau (r(2) = 0.36) and a similar positive relationship between STHg and atmospheric total Hg deposition (r(2) = 0.24). A multiple linear regression involving both variables better model the observed STHg (r(2) = 0.42). We conclude that SOC and atmospheric deposition influence STHg simultaneously in this region. The data provides information to quantify the size of the soil Hg pool in the Tibetan Plateau further, which has important implications for the Hg cycles in the permafrost regions as well as on the global scale. (C) 2020 Elsevier Ltd. All rights reserved.