Understanding the role of the unsaturated zone in aquifer recharge and contaminant attenuation processes is a major challenge for the protection and management of karstic water resources. We present the potential of the magnetic resonance soundings (MRS) geophysical method for characterizing the vadose zone of karst aquifers composed of epikarst and infiltration layers. To investigate the hydraulic functioning of the Durzon karst system located on the Larzac plateau (southern France), we used the MRS method at 16 sites. The MRS results have been compared with available geologic information and to core water content measurements. The remarkable spatial variability of the MRS response observed in the study area makes it possible to determine ranges of water storage properties in relation to the lithology of the investigated carbonate formations (dolomite, marly, and siliceous limestone). All soundings found either constant or increasing MRS water content with depth, which demonstrates that the infiltration zone might be the major water storage entity for permanent water storage, with important consequences for recharge quality and quantity. These results show the feasibility and potential of the MRS method for the characterization of the karst unsaturated zone and for understanding the vertical distribution of water content, which impacts the overall functioning of karst systems.