This dataset comprises samples collected from the Marine Atmospheric Boundary Layer (MABL) during 3 research expeditions: the 2016 summer Arctic research cruise (74 surface seawater samples), the 2017 summer Arctic research cruise (16 atmospheric and 16 surface seawater samples), and the 2016-2017 Antarctic research cruise (40 atmospheric and 34 surface seawater samples). The sampling locations encompassed various regions, including the East China Sea to Northwest Pacific transect, the Arctic Ocean region, the East China Sea to India Ocean transect, the South Ocean, and the Antarctic offshore region. The samples were analyzed for 39 semi-volatile organic compounds (SVOCs), which included polycyclic aromatic hydrocarbons (PAHs), organochlorine pesticides (OCPs), and current-use pesticides (CUPs). All samples were collected using High-volume solid phase extraction and high throughput in situ ultrasound analysis. This dataset is the Supporting Information of the research article: “Global Geographical Redistribution and Source Dynamics of SVOCs in the Marine Air Boundary Layer”, Zheng et al., 2023. The unauthorized use of this database is prohibited.