Global energy needs continue to rise along with society’s desire for carbon-reduced energy sources to limit climate change effects. One viable carbon-reduced energy source is nuclear power, which provides more than half the electricity requirements of the province of Ontario. Within Canada there are more than 2.5 million bundles of spent nuclear fuel, which will be stored in a deep geological repository. Efficiency of the repository system depends on dissipation of thermal energy. A comprehensive experimental study is presented on thermal properties of barrier materials. The influence of bentonite type, variability, moisture, and temperature on thermal properties is examined. Results show strong influence of moisture on thermal properties, some influence of temperature on low-density bentonite, minor influence of bentonite type, as well as low variability in the experimental measurements. The extensive database of physical measurements is compared with values from the literature and then used to statistically evaluate thermal property models selected from the literature. Using the base parameters from the literature, thermal property models performed adequately; however, soil-specific calibration of the model inputs improved the fit significantly. These results are now available to perform the numerical models for the proposed Canadian deep geological repository for used nuclear fuel.