The rapidity of climate change in the polar regions underscores the need for improved understanding of its impacts on ocean circulation at both regional and global scales. Reconstructions of past polar ocean-cryosphere interactions can provide this context, but large uncertainties in existing proxies limit the utility of such studies. For instance, there are currently no low-temperature (<9 °C) culture-based Mg/Ca-calibrations for planktic foraminifera, a key tool for reconstructing past changes in ocean temperatures. There is also limited understanding of non-thermal influences on Mg/Ca in <em>Neogloboquadrina pachyderma,</em> the only modern polar planktic foraminifera. Moreover, this species exhibits considerable levels of heterogeneity in composition precipitating a thick lower-Mg/Ca outer crust over higher Mg/Ca inner lamellae calcite; specimens with predominantly, albeit variable crust–lamellae proportions, are thus thought to introduce substantial uncertainty into high-latitude palaeotemperature reconstructions. Here, we used <em>N. pachyderma </em>cultured across a range of temperatures, salinities, and carbonate chemistry conditions including experiments in which pH and [CO<sub>3</sub><sup>2-</sup>] either covaried or were decoupled. By using a laser ablation approach to analyse crust and lamellae separately, we present new Mg/Ca-temperature calibrations for each component that extend culture-based calibrations in <em>N. pachyderma</em> down to the lower temperature-range (2–9 °C). The crust-specific calibration is of particular importance in high-latitude downcore records where <em>N. pachyderma</em> are commonly observed to preserve predominantly or only crust. Our results show significant carbonate chemistry influence on Mg/Ca with opposite influences from pH and carbonate ion concentration, when these variables changed in isolation. Additionally, we show that environmental conditions regulate crust-lamellar proportions, where increased salinity and temperature, and lower pH lead to less crust formation with implications for future ocean acidification and Arctic Atlantification, and for downcore reconstructions.