Vegetation structure in vast semi-arid to temperate continental land masses, such as Australia, plays a considerable role in global terrestrial carbon sequestration. However, whether soil carbon from these regions is a net atmospheric carbon source or sink remains contentious, introducing large uncertainties on long-term storage of vegetation-sequestered carbon dioxide. We investigate the interplay between catchment erosion quantified using uranium isotopes, vegetation (pollen), catchment carbon cycling, wetland response (diatoms), and lake carbon accumulation on glacial-interglacial timescales in south-eastern Australia. The analyses are applied to sediments from Lake Couridjah, in the Sydney Basin during the last (133.5 ka to 107.6 ka) and current (17.8 cal ka BP to present day) glacial-interglacial transitions. Robust phase-relationships between catchment erosion, vegetation composition and carbon cycling during both glacial-interglacial periods were revealed by statistical analyses. Vegetation structure had a direct control on catchment erosion, and, thus, on soil organic carbon (SOC) erosion in the catchment. Overall wetter and warmer peak interglacial conditions promoted the expansion of a canopy and mid-storey vegetation cover reducing catchment erosion, while simultaneously increasing SOC storage, catchment and lake primary productivity, and lake carbon storage. The results suggest increased terrestrial carbon sequestration in temperate Australian landscapes in warmer and wetter climates. • Novel trace metal isotope method quantifies “palaeo-sediment residence times” as proxy for catchment erosion • First continuous catchment erosion record for the last and current glacial-interglacial cycle in SE Australia • Link between catchment vegetation cover and erosion highlights the role of Australia as global carbon sink