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This paper aims to provide a baseline for conservation planning by documenting patterns of plant diversity and vegetation in the upper catchment of the Cuito River. 417 species are recorded from this region. Nine of these are species potentially new to science. Ten species are newly recorded from Angola, with an additional species only recorded previously within Angola from the northern enclave of Cabinda. The 108 new provincial records for Moxico clearly indicate the lack of collections from Angola’s largest province. We note the existence of extensive peat deposits in the Cuito river system for the first time and suggest that one of Barbosa’s vegetation types in the area needs to be reassessed.