The performance of high-frequency ground-penetrating radar (GPR) for high-resolution imaging of the near surface can essentially be controlled by the soil electromagnetic (EM) properties. One of these properties influencing sensing depth and image resolution of GPR is the intrinsic attenuation. We investigated the frequency-dependent electrical and dielectric properties of a broad range of soil samples. In order to derive the effective complex dielectric permittivity between 1 MHz and 10 GHz, we applied the coaxial transmission line (CTL) technique. A generalized dielectric response model, consisting of one Debye and one Cole-Cole type relaxation and a constant low-frequency conductivity term was used to analyze the dielectric relaxation behavior. Splitting the spectra into individual loss processes shows that dielectric relaxation mechanisms play a crucial role in most natural soils. Especially for high-frequency applications, attenuation cannot be described by a dielectric constant and dc-conductivity alone. Therefore, a simple conductivity-attenuation relation without dielectric losses can highly overestimate the GPR performance. As an alternative to the CTL technique in the lab, we suggest to use time-domain reflectometry (TDR) for the in Situ assessment of high-frequency electrical properties and deduced prediction of GPR performance.