We present a simple, quick, and high-resolution (approx.10 cm) method for calculating almost continuous calciumcarbonate (CaCO3) proxy records in deep-marine sediment cores based on the well-known dependence of NGR (natural gamma ray) on sediment clay content. The method used in this study is based on the assumption that sediment composition along the SAT (South Atlantic Transect) consists of two components: carbonate and clay. This assumption is reasonably accurate for the region under investigation. At carbonate-rich Site U1583 (66–97 wt% CaCO3), calculated CaCO3 wt% contents are within 4.18% at 1 standard deviation (r) of geochemical analyses of the CaCO3 wt% contents of discrete samples (measured using a coulometer), while at the more lithologically variable Site U1557 (0.1–92 wt% CaCO3), they are within 15.6% at 1r. Results indicate good to excellent correlations between the NGR- and coulometry-derived datasets, supporting the use of this method for carbonate stratigraphy, paleoceanography, and paleoclimate reconstructions. We provide an equation to derive CaCO3 wt% from NGR based on the SAT datasets. The procedure described below can be used to construct the higher resolution proxy CaCO3 records at other sites worldwide compared to discrete CaCO3 values. This method can assist with shipboard lithology determination and can guide core sampling.