Ground-penetrating radar (GPR) is a powerful tool that is still being developed for archaeological investigations. We investigated the dielectric properties of mammoth bone and bone from modern bison, cow, deer, and elk as a proxy for applying GPR for detecting prehistoric animal remains. Sample dielectric properties (relative permittivity, loss factor, and loss-tangent values) were measured with an impedance analyzer over frequencies ranging from 10 MHz to 1 GHz. Bone-sample porosity, bulk density, water saturation, and volumetric water content of the specimens were also measured. The measured sample-relative permittivity values were then compared with modeled relative permittivity values using common dielectric-mixing models to determine which parameters control the best-fit predictions of relative permittivity of animal bone. We observe statistically significant dielectric-property differences among different animal fauna, as well as variation as a function of frequency. In addition, we determine that the relative permittivity values of 8–9 for similar minerals, such as apatite, are not suitable as a proxy for predicting animal bone properties. We estimate new relative permittivity values of 3–5 for dry animal bone minerals in the frequency range of 100–1000 MHz using these common dielectric-mixing models. We postulate that differences in bone microstructure contribute to dielectric-property variability.