Secondary ion mass spectrometry (SIMS) is useful for measuring Mg/Ca in both primary calcite and diagenetic minerals in planktonic foraminifera. The excellent spatial resolution (<10 μm) and small amount of material removed (<2 ng) makes it easy to avoid targets that include obvious embedding material and encrusting or infilling minerals such as secondary calcite and authigenic clays in diagenetically altered samples. Because analyses can be performed on individuals, SIMS is also a viable technique for generating Mg/Ca values from sediment samples in which foraminifera are rare or have low mass. For clean primary calcite samples, Mg/Ca ratios from SIMS compare well to those obtained using inductively coupled plasma mass spectrometry (ICP-MS), while maintaining information regarding the true variability of elemental ratios within individual tests. For samples with secondary calcite or stubbornly adhering clays, SIMS enables us to accurately measure primary calcite compositions and to assess and reconcile contamination problems in bulk samples analyzed by solution-based ICP-MS. We have observed that SIMS is an invaluable and reliable tool for the identification and avoidance of problems of diagenesis and the analysis of rare or delicate planktonic foraminifera. However, because of operator time required to properly target delicate (thin-walled) or contaminated planktonic foraminifera, SIMS may not be feasible for Mg/Ca studies where large numbers (hundreds) of samples must be processed and bulk measurements on multiple individuals will suffice.