Accurately characterizing net evasion of elemental mercury (Hg(0)) from marine systems is essential for understanding the global biogeochemical mercury (Hg) cycle and the pool of divalent Hg (Hg(II)) available for methylation. Few high resolution measurements of Hg(0) are presently available for constraining global and regional flux estimates and for understanding drivers of spatial and temporal variability in evasion. We simultaneously measured high-resolution atmospheric and surface seawater Hg(0) concentrations as well as the total Hg distribution during six cruises in the West Atlantic Ocean between 2008 and 2010 and examined environmental factors affecting net Hg(0) formation and evasion. We observed the lowest fraction of Hg as Hg(0) (7.8±2.4%) in the near-coastal and shelf areas that are influenced by riverine inputs. Significantly higher %Hg(0) observed in open ocean areas (15.8±3.9%) may reflect lower dissolved organic carbon (DOC) in offshore environments, which is known to affect both the reducible Hg(II) pool and redox kinetics. Calculated Hg(0) evasion changed by more than a factor of three between cruises (range: 2.1±0.7- 6.8±5.1 ng m(-2) h(-1)), driven mainly by variability in Hg(0) and wind speed. Our results suggest that further mechanistic understanding of the role of DOC on Hg redox kinetics in different types of marine environments is needed to explain variability in Hg(0) concentrations and improve global estimates of air-sea exchange.