The Missão de Biologia Marítima (Lisboa, Portugal) and its successor institutions, were responsible for conducting oceanographic campaigns in former Portuguese colonies during the decades of 1950–1960. The primary objective was to advance the systematic study of marine resources in these territories, leading to the collection of thousands of specimens of marine fauna, particularly fishes, molluscs and crustaceans. In the late 1970s, the collection faced understaffing and was neglected, becoming largely inaccessible to the scientific community. This paper presents a comprehensive review of the collection, which is currently deposited in the Museu Nacional de História Natural e da Ciência, Universidade de Lisboa. The collection includes 7305 occurrences, for a total of over 30,000 specimens, most of which were collected in Angola, Cabo Verde and Mozambique between 1951 and 1965. The collection holds representatives of more than 1000 species and has a wide taxonomic coverage, including 19 type specimens of nine nominal taxa: the fishes Cubiceps niger Nümann in Franca, 1957, Tylosurus acus rafale Collete & Parin, 1970 and Chromis lubbocki Edwards, 1986; the cone snails Conus angolensis Paes da Franca, 1955 and Conus lucirensis Paes da Franca, 1955; the ark clam Arca geissei angolensis Paes da Franca, 1955; the squids Moroteuthis robsoni Adam, 1962 and Todarodes sagittatus angolensis Adam, 1962; and the snapping shrimp Alpheus holthuisi Ribeiro, 1964. A comprehensive description of the resulting dataset is provided, as well as a brief account of the history of these campaigns and the research conducted.