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Surface seawater and lower atmosphere gas samples were collected simultaneously between 18°N and 40°S in the open Pacific Ocean in 2006–2007. Samples were analyzed for organochlorine pesticides (OCPs) to assess their distribution patterns, the role of ocean in the long-range transport (LRT), and the air-water exchange directions in the open Pacific Ocean. Such open ocean studies can yield useful information such as establishing temporal and spatial trends and assessing primary vs secondary emissions of legacy OCPs. Target compounds included hexachlorocyclohexanes (HCHs), dichlorodiphenyltrichloroethanes (DDTs) and its derivatives, and chlordane compounds. Concentrations for α-HCH, γ-HCH, trans-chlordane (TC), and cis-chlordane (CC) were higher in the Northern Hemisphere (NH) than the Southern Hemisphere (SH) in both gaseous and dissolved phases, while the distribution patterns of DDTs and heptachlor exo-epoxide (HEPX) showed a reversed pattern. In the N Pacific, concentrations of α-HCH and γ-HCH in the present work were lower by 63 and 16 times than those observed in 1989–1990. The distribution patterns of DDT suggested there was usage in the SH around 2006. Calculated fugacity ratios suggested that γ-HCH was volatilizing from surface water to the atmosphere, and the air-water exchange fluxes were 0.3–11.1 ng m−2 day−1. This is the first field study that reported the open Pacific Ocean has become the secondary source for γ-HCH and implied that ocean could affect LRT of OCPs by supplying these compounds via air-sea exchange.