A dissertation submitted to the Faculty of Science, University of the Witwatersrand, Johannesburg, in fulfilment of requirements for the degree of Master of Science. Johannesburg, 2016. / This study has explored the CVD synthesis of carbon nanofibres (CNFs) using Eskom’s waste coal fly ash as a catalyst with acetylene and hydrogen as the carbon source and carrier gas, respectively. In the process, a possible growth mechanism for these carbon nanofibres was sought. CNFs were successfully synthesised from fly ash and were found to have an average diameter of 22±7 nm. The growth mechanism of these CNFs was studied using EDS, TEM and laser Raman spectroscopy. It was observed that CNFs grew via root growth on spherical particles of fly ash and by tip growth on irregular-shaped metal oxide agglomerates. Both of these were found, through EDS analysis, to be Fe-rich. CNFs were functionalised between 2-12 h under reflux at 110 °C using a 3:1 (v/v) combination of HNO3 and H2SO4 in order to introduce functional groups onto their surfaces to act as anchors for hydrophilic reactants. The functionalisation of these CNFs was studied using TEM, laser Raman spectroscopy, ATR-FTIR spectroscopy, PXRD, BET, XRF and TGA. ATR-FTIR spectroscopy showed that some carbonyl functional groups were present on the surfaces of these CNFs after functionalisation. The functionalised CNFs (fCNFs) were then treated using a simple hydrothermal method to deposit 10% (m/m) of TiO2 nanoparticles onto their surface. This hydrothermal method employed the drop-wise addition of TiCl4 to a cold water-fCNFs mixture, which was then refluxed at 115 °C for 2-12 h. Laser Raman spectroscopy confirmed the presence of both TiO2 (phase pure anatase) and CNFs. ATR-FTIR spectroscopy provisionally revealed the presence of covalent Ti-O-C bonds. Studies where the duration of exposure to TiCl4 and the functionalisation time of CNFs were examined showed that the particle size and agglomeration of the TiO2 nanoparticles did not affect the surface area of the CNF-TiO2 hybrids significantly. However, CNF-TiO2 hybrids which were shown by TGA to have high fly ash content were observed to have low surface areas. fCNFs functionalised at 2 h had the highest surface area, at all fixed durations of exposure to TiCl4 by comparison with fCNFs which had been functionalised for longer periods. / GR2016