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Metasedimentary rocks constitute an important but comparatively poorly understood part of the Antarctic Peninsula. Herein we report single-grain U-Pb detrital-zircon ages from samples of the Trinity Peninsula and Botany Bay Groups of north-western Graham Land. All studied samples are dominated by a large and narrowly defined population of late Palaeozoic zircons. Significant early–middle Palaeozoic and minor Neoproterozoic and Mesoproterozoic sub-populations constitute the majority of pre-Carboniferous grains. These detrital-zircon age populations are consistent with sediment derivation entirely from western Gondwana sources. Despite the clear Gondwana signatures, our data suggest that the Trinity Peninsula Group province was either a parautochthonous peri-Gondwanan terrane later accreted to the Antarctic Peninsula, or a significant topographic barrier precluded voluminous sediment contributions from the interior of Gondwana. Statistical comparisons with similar metasedimentary complexes of southern South America, the South Shetland Islands and eastern New Zealand indicate a diversity of sediment provenance not previously recognized, but may provide a means to better determine the pre-break-up configuration of western Gondwana. Although insufficient to definitively restore Antarctic Peninsula components adjacent to South American complexes, some Trinity Peninsula Group samples exhibit robust affinities to the Miers Bluff Formation in the South Shetland Islands and the Duque de York and Main Range Metamorphic Complexes of the Patagonian Andes.