This study represents the first comprehensive investigation of 16 polycyclic aromatic hydrocarbons (PAHs) in the waters and sediments of Lake Ulansuhai. It explores their occurrence, sources, transport behavior, and associated risks to human health and ecosystems. The results revealed that concentrations of ∑PAHs in dissolved phase and sediment with no significant seasonal differences. In contrast, ∑PAHs concentrations in suspended particulate matter were significantly higher during the ice-free period compared to the ice period. Spatially, the northern part of Lake Ulansuhai displayed higher PAHs content. Diagnostic isomeric ratios and PMF models indicated that the PAHs were primarily derived from combustion sources. The distribution of PAHs within water-sediment demonstrated that non-equilibrium status. Fugacity calculations indicated that 2–4 rings PAHs acted as secondary sources of sediment emissions. Toxicity assessment, indicated that PAHs posed no significant carcinogenic risk to humans. Risk quotient values showed that PAHs as low to high ecological risk.