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The global oceans are known as terminal sink or secondary source for diffusive emission of organochlorine pesticides (OCPs) and selected current used pesticides (CUPs) into the overlaying atmosphere. Many pesticides have been widely produced worldwide, subsequently applied, and released into the environment. However, information on the occurrence patterns, spatial variability, and air-seawater exchange of pesticides is limited to easily accessible regions and, hence, only few studies are reported from the remote Southern Ocean. To fill this information gap, a large-scale ship-based sampling campaign was conducted. In the samples from this campaign, we measured concentrations of 221 pesticides. Both gaseous and aqueous samples were collected along a sampling transect from the western Pacific to the Southern Ocean (19.75° N-76.16° S) from November 2018 to March 2019. Twenty-seven individual pesticides were frequently (= 50%) detected in gaseous and aqueous samples. Tebuconazole, diphenylamine, myclobutanil, and hexachlorobenzene (HCB) dominated the composition profile in both phases. Spatial trends analysis in atmospheric and seawater concentrations showed a substantial level reduction from the western Pacific towards the Southern Ocean. Back-trajectory analysis showed that atmospheric pesticide concentrations were strongly influenced by air masses origins. Continental and riverine inputs are important sources of pesticides in the western Pacific and Indian Oceans. Atmospheric and seawater concentrations for the target pesticide residues in the Southern Ocean are low and evenly distributed due to the large distance from potential pollution sources as well as the effective isolation by the Antarctic Convergence (AC). Air-seawater fugacity ratios and fluxes indicated that the western Pacific and Indian Oceans were secondary sources for most pesticides emitted to the atmosphere, while the Southern Ocean was still considered to be a sink.