Fish harvested from the Pacific Ocean are a major contributor to human methylmercury (MeHg) exposure. Limited oceanic mercury (Hg) data, particularly MeHg, has confounded our understanding of linkages between sources, methylation sites, and concentrations in marine food webs. Here we present methylated (MeHg and dimethylmercury (Me₂Hg)) and total Hg concentrations from 16 hydrographic stations in the eastern North Pacific Ocean. We use these data in combination with information from previous cruises and coupled atmospheric‐oceanic modeling results to better understand controls on Hg concentrations, distribution, and bioavailability. Total Hg concentrations (average 1.14 ± 0.38 pM) are elevated relative to previous cruises. Modeling results agree with observed increases and suggest that at present atmospheric Hg deposition rates, basin‐wide Hg concentrations will double relative to circa 1995 by 2050. Methylated Hg accounts for up to 29% of the total Hg in subsurface waters (average 260 ± 114 fM). We observed lower ambient methylated Hg concentrations in the euphotic zone and older, deeper water masses, which likely result from decay of MeHg and Me₂Hg when net production is not occurring. We found a significant, positive linear relationship between methylated Hg concentrations and rates of organic carbon remineralization (r² = 0.66, p < 0.001). These results provide evidence for the importance of particulate organic carbon (POC) transport and remineralization on the production and distribution of methylated Hg species in marine waters. Specifically, settling POC provides a source of inorganic Hg(II) to microbially active subsurface waters and can also provide a substrate for microbial activity facilitating water column methylation.