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Background The seaweed flora of Pico Island (central group of the Azores archipelago) has attracted interest of researchers on past occasions. Despite this, the macroalgal flora of the island cannot be considered well-known as published information reflects only occasional collections. To overcome this, a thorough investigation, encompassing collections and presence data recording, was undertaken. Research under the Campaigns “AÇORES/89”, “PICO/91”, “PICOBEL/2007” and “LAUMACAT/2011” covered a relatively large area (approximately 39 km2) around the island encompassing the littoral and sublittoral levels down to about 40 m. This paper improves the knowledge of the Azorean macroalgal flora at local and regional scales by listing taxonomic records and providing information on the ecology and occurrence of each species present on the island’s littoral. New information A total of 4043 specimens (including taxa identified only to genus level) belonging to 303 taxa of macroalgae are registered, comprising 197 Rhodophyta, 53 Chlorophyta and 53 Ochrophyta (Phaeophyceae). From these, 225 were identified to species level (142 Rhodophyta, 41 Chlorophyta and 42 Ochrophyta), encompassing 110 new records for the island (69 Rhodophyta, 20 Chlorophyta and 21 Ochrophyta), three Macaronesian endemisms (Botryocladia macaronesica Afonso-Carillo, Sobrino, Tittley & Neto; Laurencia viridis Gil-Rodríguez & Haroun; and Codium elisabethiae O. C. Schmidt), 14 introduced, and 25 species with an uncertain status. Introduction The Azorean algal flora, considered cosmopolitan with species shared with Macaronesia, North Africa, the Mediterranean Sea, Atlantic Europe and America (Tittley 2003, Tittley & Neto 2006, Wallenstein et al. 2009), has been considered relatively rich when compared to that of other remote oceanic islands (Neto et al. 2005; Tittley & Neto 2005; Wallenstein et al. 2009). Even so, it is worth mentioning that the published information (approximately 400 species, Freitas et al. 2019) reflects data from only a few of the nine islands, since not all of them have been thoroughly investigated. To overcome this, and improve the understanding of the archipelago’s seaweed flora, an effort has been made by local investigators over the past three decades and research on the marine macroalgae flora has been conducted on several of the less studied Azorean islands. This paper comprises both physical and occurrence data and compiles the gathered information from macroalgae surveys developed in Pico Island mainly by the Island Aquatic Research Group of the University of the Azores (https://ce3c.ciencias.ulisboa.pt/sub-team/island-aquatic-ecology). It aims to constitute a practical resource for biological studies such as systematics, diversity and conservation, biological monitoring, climate change and ecology, and also for academics, students, government, private organizations, and the general public. Purpose By listing taxonomic records for Pico and presenting general information for each taxon occurrence on the island’s littoral, this paper addresses several biodiversity shortfalls (see Hortal et al. 2015), namely the need to catalogue the Azorean macroalgae (Linnean shortfall) and improve the current information on their local and regional geographic distribution (Wallacean shortfall), as well as on species abundances and dynamics in space (Prestonian shortfall).