Accelerated erosion of fine-grained sediment is an environmental problem of international dimensions. Erosion control strategies and targeting of mitigation measures require robust and quantitative identification of sediment sources. Here, we use magnetic ‘fingerprinting’ to characterize soils, and examine their affinity with and contribution to suspended sediments transported within two subcatchments feeding Bassenthwaite Lake, northwest England. A high-resolution soil magnetic susceptibility survey was made using a field susceptometer (ZH Instruments, SM400 probe). Combining the spatial and vertical (down-profile) soil magnetic data, a subset of soil profiles was selected for detailed, laboratory-based magnetic remanence analyses. The magnetic properties of the catchment soils are highly particle size-dependent. Magnetic analyses were performed on the 31–63 μm fraction, for particle size-specific comparison both with the suspended sediments and lake sediments. Fuzzy cluster analysis groups the soil magnetic data into six clusters, apparently reflecting variations in parent material and horizon type, with three magnetically hard soils as unclassified outliers. Examination of the cluster affinity of the soils, suspended sediments and lake sediments indicates that topsoils of the upper Newlands Valley and subsoils around Keskadale Beck are a major source of the Newlands Beck suspended load, and the recent (post-nineteenth century) sediments in the deep lake basin. Older lake sediments show strong affinity with a small number of the Derwent suspended sediments and one of the Glenderamackin soils. A large number of Derwent suspended sediments show no affinity with any of the soils or lake sediments, instead forming a coherent, discrete and statistically unclassified group, possibly resulting from mixing between the magnetically hard subsoils of the medium to high-altitude Glenderamackin and Troutbeck areas and softer, lower altitude Glenderamackin soils. The lack of any affinity of these suspended sediments with the lake sediments may indicate deposition along the Derwent flood plain and/or in the shallow delta of Lake Bassenthwaite. Particle size-specific magnetic fingerprinting is thus shown to be both highly discriminatory and quantitatively robust even within the homogeneous geological units of this catchment area. Such a methodological approach has important implications for small–large scale catchment management where sources of sediment arising from areas with uniform geology have been difficult to determine using other approaches, such as geochemical or radionuclide analyses.