Coccolithophores have been extensively studied to understand the environmental control on calcification in a key biological group influencing the alkalinity of seawater. Previous studies have established that bulk calcification scales with cell division rates under a wide range of pH conditions. Yet the fine-scale ultrastructural changes of the coccoliths and therefore the pH-sensitive underlying mechanisms altering biomineralization of the coccoliths remain largely underconstrained. Using circularly polarized light and high-resolution microscopy, we have generated mass estimates of cultured Gephyrocapsa oceanica coccoliths grown in media with pH values ranging from 7.4 to 9.0. These mass estimates representing a bulk calcification response were related to the morphological changes within the coccoliths. From optimal (pH 8.6) down to pH 7.4 conditions, we have observed that impaired cell growth and lower calcite quota are accompanied by a 35% decrease in mean coccolith mass. The data further show that seawater acidification does not homogenously affect calcification of the coccoliths, as a clear decrease of the breadth of the tube (a structure surrounding the central area of the coccoliths) was detected, whereas all other ultrastructural components were far less impacted. We discuss this specific sensitivity to acidification as the possible consequence of the altered interaction of the acidic polysaccharides used for biomineralization and ambient concentration of protons released by calcification that substantially modify the growth patterns, the morphology, and ultimately the mass of the coccoliths.Plain Language Summary Anthropogenic rise in CO 2 concentrations induces ocean acidification, which represents a threat for marine organisms. As calcium carbonate is sensitive to pH, those organisms secreting calcite shells, such as the coccolithophores (unicellular microalgae), are particularly exposed to ongoing climate change. Previous studies have documented that the coccoliths, the calcite biominerals produced intracellularly by the coccolithophores, will be adversely affected by decreased ambient pH values. Yet how this reduction operates at the scale of the coccolith remains elusive and we are thus lacking an understanding of the intracellular mechanisms behind undercalcification, which is essential to anticipate the response of marine calcifiers in a changing planet. We analyzed the morphometric parameters of coccoliths grown under the pH range 7.4-9.0. Our data show a clear reduction in coccolith mass in more acidic conditions, and we explain this change by altered growth of calcite at an early stage of the formation of the biomineral. This study suggests that certain organic molecules used to promote intracellular calcification are perturbed by decreased local pH and that less calcified coccoliths produced within the cell cannot be the result of a postmortem process that may occur when calcite is bathed in relative low-pH environments after their secretion outside the cells.