We combine geophysical observations from ground-penetrating radar (GPR) with regolith physical and chemical properties from pedons excavated in four study areas spanning 1300 km of the climate and ecological gradient in the Chilean Coastal Cordillera. Our aims are the following: (1) to relate GPR observations to depth-varying regolith physical and weathering-related chemical properties in adjacent pedons and (2) to evaluate the lateral extent to which these properties can be extrapolated along a hillslope using GPR observations. Physical observations considered include regolith bulk density and grain size distribution, whereas chemical observations are based on major and trace element analysis. Results indicate that visually determined pedolith thickness and the transition from the B to C horizons generally correlate with maximums in the 500 and 1000MHz GPR envelope profiles. To a lesser degree, these maximums in the GPR envelope profiles agree with maximums in weathering-related indices such as the chemical index of alteration (CIA) and the chemical index of mass transfer (τ) for Na. Finally, we find that upscaling from the pedon to hillslope scale is possible with geophysical methods for certain pedon properties. Taken together, these findings suggest that the GPR profiles down hillslopes can be used to infer lateral thickness variations in pedolith horizons in different ecologic and climate settings, and to some degree the physical and chemical variations with depth.