Mercury (Hg) in aquatic ecosystems is of great concern due to its toxicity, bioaccumulation, and magnification in the food web. The Tibetan Plateau (TP) is endowed with the highest and largest lakes on earth, whereas Hg distribution and behavior in lake waters are least known. In this study, surface water samples from 38 lakes over the TP were collected and determined for the total Hg (THg) concentrations. Results revealed a wide range of THg concentrations from <1 ng to 40.3 ng L(-1). THg in lake waters exhibited an increasing trend along the southeast to northwest transect over the TP. Strong positive correlations were observed between THg concentrations and salinity and salinity-related environmental variables, especially for total dissolved solids (TDS) and some of the major ions such as Na(+), K(+), and Cl(-), suggesting the enrichment of Hg in saline lakes. The large-scale geographical pattern of climatic and environmental factors shows a decreasing precipitation and an increasing evaporation northwards and westwards and thereby induces gradient-enhanced enrichment of soluble substances in lake waters, which are likely to complex more Hg in northwestern TP. Our study provides the first comprehensive baseline data set of Hg in Tibetan lake waters and highlights the concurrent high Hg and salinity, representing valuable references and fundamental rules in further understanding the behavior and fate of Hg in lakes over the TP and perhaps high-altitude regions beyond.