Three nuclear weapons tests were conducted in the 1950s at the Montebello Islands, Western Australia. The detonations were of different yields and configurations (two tower tests, one ship test), and led to substantial radionuclide contamination within the surrounding terrestrial and marine ecosystems. The region possesses great ecological and recreational significance, particularly within the marine environment. However, studies conducted so far have largely neglected the marine ecosystem which makes up the majority of the Montebello Island Marine Park and in which most test fallout would have deposited. Here we investigated the distribution of the transuranic radionuclides 238Pu, 239,240Pu and 241Am in marine sediment from the Montebello Islands. Marine sediment samples near Operation Mosaic G2 and Operation Hurricane were collected and analysed by gamma and alpha spectrometry. Activity concentrations of 239,240Pu across both series ranged from 45 to 2900 Bq kg−1, while 241Am levels ranged from 2.8 to 70 Bq kg−1. Higher activity concentrations were observed in sediment near the land-based, higher yield Mosaic G2 test, compared with the ship-based, lower yield Hurricane test. Sediment samples located closer to the detonation site were also observed to have higher activity concentrations. Radioactive particles of 0.94 mm and 1.5 mm in diameter were identified by analysis of size-fractioned sediment via investigation of 152Eu levels, photostimulated autoradiography and point gamma spectroscopy. Particles were confirmed to have transuranic radionuclide interiors, with surface coatings which were dominated by vitrified CaCO3. Their long-term resistance to weathering and subsequent persistence in the marine environment can therefore be attributed to their coated structural form. Our study confirms the persistence of transuranic radionuclides in Montebello Island marine sediment and highlights the need for additional studies to improve our understanding of the nuclear legacy in this region.