Natural gamma-ray measurements were made in the GSC Smeaton drillhole as part of the borehole geophysical classification of kimberlite pipe 169. In addition, forty samples of Cretaceous sediments (shales, siltstones, and sandstones) and thirty-five kimberlite samples, selected from the drill core, were analyzed for major and trace elements. These elements included potassium (K), uranium (U), and thorium (Th), which are the main naturally-occurring radioactive elements. Different phases of the kimberlite, and the Cretaceous sediments which show variations in the gamma-ray activity, can be easily delineated on the gamma-ray logs. The gamma-ray logs indicate that the radioactivity in the kimberlite derives mainly from Th, and, to a lesser extent, U. Most of the kimberlite units are enriched in Th and U relative to the Cretaceous sediments, and these radioelements are mainly hosted by accessory apatite and perovskite, and minor zircon. Potassium concentrations are low in the kimberlite. The higher K concentration in the sediments clearly distinguishes the Cretaceous sediments from the kimberlite. The U/K and Th/K ratios show important and distinct differences between the two major types of volcaniclastic kimberlite. Kimberlite lapillistones have higher U/K and Th/K ratios than the olivine crystal tuffs. Furthermore, standardized U/K and Th/K geophysical logs can be used to separate marine reworked olivine shoreface sands from other shallow marine sediments that contain kimberlitic detritus. The identification of different phases and/or stratigraphic facies of kimberlite on the basis of radioelement distributions means that gamma-ray spectrometry can assist exploration, particularly in regard to diamond grade distribution.