The magnesium/calcium ratio (Mg/Ca) and calcium (Ca) concentration of seawater have oscillated throughout geologic time; our experiments indicate that these variables have strongly influenced biomineralization and chalk production by coccolithophores. The high Mg/Ca ratio of modern seawater favors precipitation of high-Mg calcite and/or aragonite. In contrast, the low Mg/Ca ratio of imputed Cretaceous seawater favored precipitation of low-Mg calcite. We have discovered that some coccolithophore species today secrete skeletal elements of high-Mg calcite, rather than low-Mg calcite, as conventionally believed. These species incorporated less Mg when the ambient Mg/Ca ratio was lowered, secreting low-Mg calcite in imputed Cretaceous seawater. Calcification stimulates cocco lithophore population growth by contributing CO2 to photosynthesis. Three extant coc co lithophore species multiplied much faster as the composition of ambient seawater was shifted toward that estimated for Cretaceous seas. Two of these species secreted high-Mg calcite in ambient seawater having Mg/Ca > 1, and incorporation of Mg in a calcite crystal inhibits growth. Calcification of the third species, which secreted low-Mg calcite at all ambient Mg/Ca ratios, is hindered by the high Mg/Ca ratio and low absolute concentration of Ca of modern seawater. We conclude that the ionic composition of Cretaceous seawater enabled cocco lithophores to produce massive chalk deposits, and conversely, that the ionic composition of modern seawater inhibits population growth for most extant coccolitho phore species, which occupy nutrient-poor waters and fail to respond to fertilization by nitrate, phosphate, or iron.