The pervasive use of computer-generated graphics in our society has led to strict demands on their visual realism. Generally, users of rendering software want their images to look, in various ways, "real", which has been a key driving force towards methods that are based on the physics of light transport. Until recently, industrial practice has relied on a different set of methods that had comparatively little rigorous grounding in physics-but within the last decade, advances in rendering methods and computing power have come together to create a sudden and dramatic shift, in which physics-based methods that were formerly thought impractical have become the standard tool. As a consequence, considerable attention is now devoted towards making these methods as robust as possible. In this context, robustness refers to an algorithm's ability to process arbitrary input without large increases of the rendering time or degradation of the output image. One particularly challenging aspect of robustness entails simulating the precise interaction of light with all the materials that comprise the input scene. This dissertation focuses on one specific group of materials that has fundamentally been the most important source of difficulties in this process. Specular materials, such as glass windows, mirrors or smooth coatings (e.g. on finished wood), account for a significant percentage of the objects that surround us every day. It is perhaps surprising, then, that it is not well-understood how they can be accommodated within the theoretical framework that underlies some of the most sophisticated rendering methods available today. Many of these methods operate using a theoretical framework known as path space integration. But this framework makes no provisions for specular materials: to date, it is not clear how to write down a path space integral involving something as simple as a piece of glass. Although implementations can in practice still render these materials by side-stepping limitations of the theory, they often suffer from unusably slow convergence; improvements to this situation have been hampered by the lack of a thorough theoretical understanding. We address these problems by developing a new theory of path-space light transport which, for the first time, cleanly incorporates specular scattering into the standard framework. Most of the results obtained in the analysis of the ideally smooth case can also be generalized to rendering of glossy materials and volumetric scattering so that this dissertation also provides a powerful new set of tools for dealing with them. The basis of our approach is that each specular material interaction locally collapses the dimension of the space of light paths so that all relevant paths lie on a submanifold of path space. We analyze the high-dimensional differential geometry of this submanifold and use the resulting information to construct an algorithm that is able to "walk" around on it using a simple and efficient equation-solving iteration. This manifold walking algorithm then constitutes the key operation of a new type of Markov Chain Monte Carlo (MCMC) rendering method that computes lighting through very general families of paths that can involve arbitrary combinations of specular, near-specular, glossy, and diffuse surface interactions as well as isotropic or highly anisotropic volume scattering. We demonstrate our implementation on a range of challenging scenes and evaluate it against previous methods.