Current treatments for diseases and trauma of dental and oral structures rely on durable materials such as amalgam and synthetic materials, or autologous tissue grafts. A paradigm shift has taken place in utilising electrospun nanofibres for tooth restoration and dento-oral regeneration. Use of electrospun fibres and their scaffolds in dento-oral applications involves several considerations, including choice of material, fibre orientation, porosity, surface modification and tissue application. Choices of materials include both natural and synthetic materials and a combination of both and the surface of the scaffold can be modified by osteoconductive components, which can provide an optimal combination of mechanical and biomimetic properties. This chapter highlights recent advances in the application of electrospun nanofibres in dentistry, including the tooth restoration and periodontium regeneration with specific emphasis on resin matrix interaction, cells, biomaterial matrix scaffolds and integrated tissue engineering approaches. © 2011 Woodhead Publishing Limited. All rights reserved.