The work carried out for this thesis focussed on four main areas: (i) the examination and optimisation of the conditions for carbon nanofibre (CNF) growth, both unsupported and as films on substrates; (ii) the electrochemical characterisation of the CNF material before (as-grown) and after solubilisation (oxidation); (iii) the formation and investigation of CNF thin film electrodes; and (iv) the (co-)deposition of the CNFs with metals from aqueous plating solutions. CNFs are grown at an iron nanoparticle catalyst produced from an iron oxide precursor. After exploratory work with different types of iron oxide precursors, a suitable and universally applicable catalyst is identified. CNFs are characterised by electron microscopy, spectroscopy, and electrochemistry. When grown onto a ceramic substrate, the 'as-grown' CNF material is shown to act as a porous, high surface area electrode with the ability to strongly adsorb aromatic molecules, such as hydroquinone, benzoquinone, and phenol.