Methylmercury (MeHg) concentrations can increase by 100 000 times between seawater and marine phytoplankton, but levels vary across sites. To better understand how ecosystem properties affect variability in planktonic MeHg concentrations, we develop a model for MeHg uptake and trophic transfer at the base of marine food webs. The model successfully reproduces measured concentrations in phytoplankton and zooplankton across diverse sites from the Northwest Atlantic Ocean. Highest MeHg concentrations in phytoplankton are simulated under low dissolved organic carbon (DOC) concentrations and ultraoligotrophic conditions typical of open ocean regions. This occurs because large organic complexes bound to MeHg inhibit cellular uptake and cell surface area to volume ratios are greatest under low productivity conditions. Modeled bioaccumulation factors for phytoplankton (102.4-105.9) are more variable than those for zooplankton (104.6-106.2) across ranges in DOC (40-500 μM) and productivities (ultraoligotrophic to hypereutrophic) typically found in marine ecosystems. Zooplankton growth dilutes their MeHg body burden, but they also consume greater quantities of MeHg enriched prey at larger sizes. These competing processes lead to lower variability in MeHg concentrations in zooplankton compared to phytoplankton. Even under hypereutrophic conditions, modeled growth dilution in marine zooplankton is insufficient to lower their MeHg concentrations, contrasting findings from freshwater ecosystems. © 2017 American Chemical Society.