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Abstract We investigate the origin and fate of lithogenic sediments using magnetic mineral assemblages in Barilari Bay, west Antarctic Peninsula (AP) from sediment cores recovered during the Larsen Ice Shelf System, Antarctica (LARISSA) NBP10‐01 cruise. To quantify and reconstruct Holocene changes in covarying magnetic mineral assemblages, we adopt an unsupervised mathematical unmixing strategy and apply it to measurements of magnetic susceptibility as a function of increasing temperature. Comparisons of the unmixed end‐members with magnetic observations of northwestern AP bedrock and the spatial distribution of magnetic mineral assemblages within the fjord, allow us to identify source regions, including signatures for “inner bay,” “outer bay,” and “northwestern AP” sources. We find strong evidence that supports the establishment of a late Holocene ice shelf in the fjord coeval with the Little Ice Age. Additionally, we present new evidence for late Holocene sensitivity to conditions akin to positive mean Southern Annual Mode states for western AP glaciers at their advanced Neoglacial positions.