During root canal treatment, the root canal of a tooth is prepared, disinfected and filled. Alkaline materials have been used in endodontics for many years mainly as medicament pastes rather than for obturation of the root canal system. Calcium hydroxide, the most commonly used alkaline material in dentistry, releases hydroxyl ions which cause disinfection of the root canal system. The first part of this thesis examines the use of calcium hydroxide in non-aqueous solvents and compares this to calcium hydroxide in traditional water-based solvents. The novel use of anthocyanin as an indicator allowed tracking of diffusion of hydroxyl ions through root dentine.The discovery of calcium hydroxide-induced polymerisation of certain organic compounds such as glycerol to form a hard setting alkaline cement opens the possibility of using these materials for short or long term obturation of the root canal. In the second part of the thesis, a bacterial leakage study was carried out to compare the sealing capabilities of various root filling materials including this novel hard-setting alkaline cement as well as mineral trioxide aggregate (MTA) cements, which release calcium hydroxide from their setting reaction, and traditional epoxy resin sealers.In the third part of the thesis, the root fillings were then assessed in terms of their removability, a parameter which is relevant both for post space preparation and in the event that retreatment is required. Materials were tagged with a fluorescent label and then confocal laser scanning microscopy was used to assess the extent of remnant material and the cleanliness of the root canal walls.The results from Part 1 indicated that hydroxyl ion release into root dentine is greater with non-aqueous solvents, resulting in a sustained level of high alkalinity within the root.This feature should provide longer disinfection and should therefore reduce the number of inter-appointment visits clinically. In Part 2, bacterial leakage studies demonstrated that alkaline cements had greater sealing capabilities than commonly used epoxy resin sealers. This is most likely due to the antibacterial actions of hydroxyl ions released from alkaline cements. In Part 3 of the thesis, with regards to removability using rotary instrumentation, the novel hard-setting calcium hydroxide cement was more easily removed than MTA 3 cements or epoxy resin sealers, with the latter coating half of the canal walls after instrumentation.Overall, the findings from this thesis show that while calcium hydroxide pastes based on water are an integral and long standing part of root canal disinfection, the potential use of calcium hydroxide in dentistry is wider than its current applications. The research from this thesis shows that calcium hydroxide in non-aqueous solvents may be suitable for use as a disinfecting medicament and that when incorporated into a cement it may have properties that are well suited to being used in obturation of the root canal.4