Through the production and export of their calcite coccoliths, coccolithophores form a key component of the global carbon cycle. Despite this key role, very little is known about the biogeochemical role of different coccolithophore species in terms of calcite production, and how these species will respond to future climate change and ocean acidification. Here, we present the first study to estimate species-specific calcite production, from samples collected in the Arctic Ocean and subarctic Iceland Basin in June 2012. We show that although the coccolithophorid Coccolithus pelagicus comprised only a small fraction of the total community in terms of abundance (2%), our estimates indicate that it was the major calcite producer in the Arctic Ocean and Iceland Basin (57% of total calcite production). In contrast, Emiliania huxleyi formed 27% of the total abundance and was responsible for only 20% of the calcite production. That C. pelagicus was able to dominate calcite production was due to its relatively high cellular calcite content compared with the other species present. Our results demonstrate, for the first time, the importance of investigating the complete coccolithophore community when considering pelagic calcite production, as relatively rare but heavily calcified species such as C. pelagicus can be the key calcite producers in mixed communities. Therefore, the response of C. pelagicus to ocean acidification and climate change has the potential to have a major impact on carbon cycling within the North Atlantic and Arctic Ocean.