In this study, we investigated the accelerating pace of anthropogenic land use and land cover change (LULCC) disturbance, which has generated enormous impacts on the Crocodile River. Spot images from 1996, 2009 and 2022 were used to generate the land use maps and quantify the changes. A supervised classification with the maximum likelihood classifier was used to classify the images. Sediment sources were classified into two sources, revealed by erosional characteristics in the catchment. A gamma spectrometry detector, high-purity germanium (HPGe) “Well” detector by Canberra and inductively coupled plasma mass spectrometry (ICP–MS) were used for the analysis of the samples. The results revealed that from 1996–2022, built-up areas, bare land and water bodies increased by 3.48%, 2.47% and 1.90%, respectively. All the LULCC classes increased annually from 1996–2022, except for grassland, which shrunk. The results of the radionuclides analysis showed that 210Pbex was found to be a more effective tracer than 137Cs. The mass balance model revealed that subsurface sources contributed 60%, while surface sources contributed 40%, of the sediment load in the river. This research provides valuable information necessary for integrated catchment management policies for future LULCC and soil erosion to be adopted.