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Atmospheric processes (air-surface exchange, and atmospheric deposition and degradation) are crucial for understanding the global cycling and fate of organic pollutants (OPs). However, such assessments over the Tibetan Plateau (TP) remain uncertain. More than 50% of Chinese lakes are located on the TP, which exerts a remarkable influence on the regional water, energy, and chemical cycling. In this study, air and water samples were simultaneously collected in Nam Co, a large lake on the TP, to test whether the lake is a secondary source or sink of OPs. Lower concentrations of organochlorine pesticides (OCPs) and polychlorinated biphenyls (PCBs) were observed in the atmosphere and lake water of Nam Co, while the levels of polycyclic aromatic hydrocarbons (PAHs) were relatively higher. Results of fugacity ratios and chiral signatures both suggest that the lake acted as the net sink of atmospheric hexachlorocyclohexanes (HCHs), following their long-range transport driven by the Indian monsoon. Different behaviours were observed in the PAHs, which primarily originated from local biomass burning. Acenaphthylene, acenaphthene, and fluorene showed volatilization from the lake to the atmosphere, while other PAHs were deposited into the lake due to the integrated deposition process (wet/dry and air-water gas deposition) and limited atmospheric degradation. As the dominant PAH compound, phenanthrene exhibited a seasonal reversal of air-water gas exchange, which was likely related to the melting of the lake ice in May. The annual input of HCHs from the air to the entire lake area (2015 km(2) ) was estimated as 1.9 kg yr(-1), while input estimated for Sigma(15)PAHs can potentially reach up to 550 kg yr(-1). This study highlights the significance of PAH deposition on the regional carbon cycling in the oligotrophic lakes of the TP.