The relationship between soil redistribution processes (i.e. soil erosion and deposition), using the caesium-137 (¹³⁷Cs) method, and the movement, storage and loss of soil organic carbon (SOC) are examined for a small catchment in south-eastern Australia. While recent studies have found strong and statistically significant relationships between ¹³⁷Cs and SOC within heavily cultivated (i.e. highly disturbed) landscapes, there has been a dearth of studies in uncultivated conditions. The site used in this study is characterized by different land use histories and soil types and therefore offers a unique opportunity to investigate the relationship between ¹³⁷Cs and SOC for both cultivated and uncultivated conditions. Depth distribution profiles and hillslope transects were sampled for ¹³⁷Cs and SOC to examine the relationship between the redistribution of soil particles and SOC at the point and hillslope scale. It was noted that the distribution of ¹³⁷Cs and SOC with depth in the soil profile differs among land use and soil types. The relationship between ¹³⁷Cs and SOC was also investigated, with results indicating that there was no relationship between ¹³⁷Cs and SOC for uncultivated hillslopes. In contrast, strong and statistically significant relationships were found for the previously cropped transects. The lack of a relationship within uncultivated hillslope areas in the current study appears to indicate that SOC and ¹³⁷Cs are not moving along the same physical pathways or by the same mechanisms, rather it is suggested that the spatial distribution of SOC is a result of biological factors (e.g. biological oxidation, mineralization). The results of this study suggest that the use of ¹³⁷Cs data to predict SOC redistribution patterns in grazing, largely undisturbed landscapes is problematic. Caution is thus required before using ¹³⁷Cs to predict the spatial distribution of SOC within uncultivated landscapes in this region of Australia, and within similar dry climatic regions.