Ph.D. (Geology) / The successions of the Cape- and Karoo Supergroups preserve an integrated history of sedimentation along the paleo-Pacific margin of Gondwana from the Paleozoic to the Early Mesozoic. The Cape- and Karoo Supergroups have been well studied with regard to stratigraphy, sedimentary facies and depositional environment. However, the nature and location of their source regions, especially for the changeover from deposition within an Atlantic-type continental margin basin for the successions of the Cape Supergroup to an Andean-type continental foreland basin for some of the units of the Karoo Supergroup, remains poorly understood. In order to shed light on the nature of these source regions, a comprehensive U-Pb detrital zircon study of the successions of the Cape- and lower Karoo Supergroups was launched. A representative number of samples from the upper and lower successions of the Table Mountain- Bokkeveld- and Witteberg Groups of the Cape Supergroup as well as the Dwyka and Ecca Groups of the Karoo Supergroup were collected throughout the western, southwestern and southern Cape region. A few samples of the Dwyka Group were also collected within the more eastern outcrop regions of the succession located in Kwazulu-Natal. The sedimentary rocks of the Natal Group and Msikaba Formation have long been regarded as coeval with the Cape Supergroup. Similar to the successions of the Cape- and Karoo Supergroups, very little is known about their sedimentary source regions. Also, their relative age of sedimentation remains poorly constrained. The U-Pb detrital zircon study of the successions of the Cape- and lower Karoo Supergroups was thus extended so as to include the successions of the Natal Group and Msikaba Formation. The detrital zircon age populations of the successions of the Natal Group and Msikaba Formation would not only improve the present understanding with regards to the sedimentary source regions to these units but would also facilitate the evaluation of possible correlations between these units and the stratigraphic units of the Cape Supergroup. Samples of both the lower Durban Formation and the upper Mariannhill Formation of the Natal Group and the Msikaba Formation (which is presently regarded as being part of the Cape Supergroup) were therefore collected within their respective outcrop regions in the Kwazulu-Natal area. The similarities in litho- and bio-stratigraphy between the successions of the Cape- and Karoo Supergroups and those of the Ordovician to Early Permian successions of the Ventania System and the Ordovician to Silurian successions of the Tandilia System in Argentina have long been recognized. Although the detrital zircon populations of some of the formations within these Systems have been evaluated in the past, it is yet to be determined whether these successions and those of the Cape- and lower Karoo Supergroups have certain source regions in common. In order to facilitate such a comparison, samples of selected units of the Ventania System were therefore collected near Sierra de la Ventania, while a sample of the Balcarce Formation of the Tandilia System was obtained near Mar del Plata. The detrital zircon age populations of the successions of the Ventania and Tandilia Systems were also further evaluated in the light of establishing or confirming a time-correlation between these formations and those of the Cape- and lower Karoo Supergroups. U-Pb age determination of the detrital zircons population of the samples was conducted by means of Laser Ablation-Inductively Coupled Plasma-Mass Spectrometry (LA-ICP-MS). Although LA-ICP-MS is a routine, well-established technique where the U-Pb age determination of detrital zircons is concerned, it was yet to be established at the centralized analytical facility of the University of Johannesburg, SPECTRUM, using the instrumentation currently available (i.e. 213nm Nd:YAG laser coupled to Quadrupole-based ICP-MS). The U-Pb age determination of detrital zircons was therefore preceded by a fair amount of instrument optimization and method development. Well studied shortcomings of U-Pb detrital zircon dating by LA-ICP-MS such as laser induced elemental fractionation, mass discrimination effects and as well as the possible occurrence of minor common-Pb needs were addressed and corrected for. The detrital zircon populations of successions in the Cape Supergroup have a distinct major Neoproterozoic to Early Cambrian age component, which can be attributed to an input of detritus from successions related to the Pan-African Orogeny in South Africa, such as the Gariep- and Saldania Belts located towards the north of the Cape Basin. A substantial amount of Mesoproterozoic detrital zircon grains is also present in all the samples from the successions of the Cape Supergroup. These grains of Mesoproterozoic age were probably derived from the Namaqua-Natal Metamorphic Province, which is also regarded as the source of some minor amounts of Paleoproterozoic detrital zircon grains. The near absence of Archean grains from the detrital zircon populations of the successions of the Cape Supergroup is notable, and is thought to be due to the Namaqua-Natal Metamorphic Province acting as a geomorphological barrier at the time of their deposition. The minor Paleozoic (Ordovician to Carboniferous) detrital zircon populations in the samples from the formations of the Cape Supergroup increase progressively upwards through the succession. ....