Methylmercury (MeHg) is known to biomagnify in marine food chains, resulting in higher concentrations in upper trophic level animals than their prey. To better understand how marine copepods, an important intermediate between phytoplankton and forage fish at the bottom of the food chain, assimilate and release MeHg, we performed a series of laboratory experiments using the gamma-emitting radiotracer 203Hg2+ and Me203Hg with the calanoid copepod Acartia tonsa. Assimilation efficiencies (AEs) of Hg2+ and MeHg ranged from 25 to 31% and 58 to 79%, respectively, depending on algal diets. The AEs were positively related to the fraction of mercury in the cytoplasm of the algal cells that comprised their diet. Efflux rates of Hg2+ (0.29/d) and MeHg (0.21/d) following aqueous uptake were similar, but efflux rates following dietary uptake were significantly lower for MeHg (0.11-0.22 /d) than Hg2+ (0.47-0.66 /d). The calculated trophic transfer factors (TTFs) in copepods were >1 for MeHg and consistently low (≤0.2) for Hg2+. We used the parameters measured in this study to (1) quantitatively model the relative importance of MeHg sources (water or diet) for copepods, and to (2) predict the overall MeHg concentrations in copepods in different marine environments. In general, MeHg uptake from diet accounted for most of the body burden in copepods (>50%). For an algal diet whose MeHg dry weight bioconcentration factor (BCF) is ≥106, over 90% of a copepod's MeHg body burden can be shown to derive from diet. Our model-predicted MeHg concentrations in the copepods were comparable to independent measurements for copepods in coastal and open-ocean regions, implying our measured parameters and model are applicable to natural waters.