This dataset holds foliar trait measurements, species-level life history traits, visible-near infrared (VNIR) spectroscopy, and vegetation survey data for plant communities within the Greater Cape Floristic Region (GCFR) of South Africa. Foliar traits measurements were made between 2010 and 2014. Releve surveys data include plots from 1966 to 2014. Trait collection efforts extended over 5.8% of the GCFR's total area, where measurements were made for 1,327 species from 99 families. The trait dataset comprises 135,325 leaf and twig structural measurements, 7,513 canopy measurements and 11,950 elemental/isotopic measurements. The spectroscopy dataset contains 3,205 VNIR spectral measurements (450-949 nm) of 1,181 species from 96 families. These data contribute to research initiatives such as the Biodiversity Survey of the Cape (BioSCape) project and help understand this ecosystem from a trait-based perspective. The data are provided in comma separated values (CSV) format.