The tufa deposits of the Ghaap Plateau escarpment provide a rich, yet minimally explored, geological archive of climate and environmental history coincident with hominin evolution in South Africa. This study examines the sedimentary and geochemical records of ancient and modern tufas from Buxton-Norlim Limeworks, Groot Kloof, and Gorrokop, to assess the potential of these sediments for providing reliable chronologies of high-resolution, paleoenvironmental information. Chronometric dating demonstrates that tufa formation has occurred from at least the terminal Pliocene through to the modern day. The stable isotope records show a trend toward higher, more variable δ18O and δ13C values with decreasing age from the end of the Pliocene onwards. The long-term increase in δ18O values corresponds to increasingly arid conditions, while increasing δ13C values reflect the changing proportion of C3/C4 vegetation in the local environment. Analysis of the Thabaseek Tufa, in particular, provides valuable evidence for reconstructing the depositional and chronological context of the enigmatic Taung Child (Australopithecus africanus). Collectively, the results of the present study demonstrate the potential of these deposits for developing high-precision records of climate change and ultimately, for understanding the causal processes relating climate and hominin evolution.