A numerical and experimental study of buoyancy-driven flow in the annulus between two horizontal coaxial cylinders at Rayleigh numbers approaching and exceeding the critical values is presented. The stability of the flow is investigated using linear theory and the energy method. Theoretical predictions of the critical Rayleigh number for onset of secondary flows are obtained for a wide range of radius ratio R and are verified by comparison with results of previous experimental studies. A subcritical Rayleigh number which provides a necessary condition for global flow stability is also determined. The three-dimensional transient equations of fluid flow and heat transfer are solved to study the manifestation of instabilities within annuli having impermeable endwalls, which are encountered in various applications. For the first time, a thorough examination of the development of spiral vortex secondary flow within a moderate gap annulus and its interaction with the primary flow is performed for air. Simulations are conducted to investigate factors influencing the size and number of post-transitional vortex cells. The evolution of stable three-dimensional flow and temperature fields with increasing Rayleigh number in a large gap annulus is also studied. The distinct flow structures which coexist in the large gap annulus at high Rayleigh numbers preceding transition to oscillatory flow, including transverse vortices at the end walls which have not been previously identified, are established numerically and experimentally. The solutions for the large-gap annulus are compared to those for the moderate-gap case to clarify fundamental differences in behaviour. Heat transfer results in the form of local Nusselt number distributions are presented for both the moderate- and large-gap cases. Results from a series of experiments performed with air to obtain data for validation of the numerical scheme and further information on the flow stability are presented. Additionally, the change from a crescent-shaped flow pattern to a unicellular pattern with centre of rotation at the top of the annulus is investigated numerically and experimentally for a Prandtl number of 100. Excellent agreement between the numerical and experimental results is shown for both Prandtl numbers studied. The present work provides, for the first time, quantitative three-dimensional descriptions of spiral convection within a moderate-gap annulus containing air, flow structures preceding oscillation in a large-gap annulus for air, and unicellular flow development in a large-gap annulus for large Prandtl number fluids.