High-performance computing increasingly occurs on “computational grids” composed of heterogeneous and geographically distributed systems of computers, networks, and storage devices that collectively act as a single “virtual” computer. A key challenge in this environment is to provide efficient access to data distributed across remote data servers. This dissertation explores some of the issues associated with I/O for wide-area distributed computing and describes an I/O system, called Armada, with the following features: a framework to allow application and dataset providers to flexibly compose graphs of processing modules that describe the distribution, application interfaces, and processing required of the dataset before or after computation; an algorithm to restructure application graphs to increase parallelism and to improve network performance in a wide-area network; and a hierarchical graph-partitioning scheme that deploys components of the application graph in a way that is both beneficial to the application and sensitive to the administrative policies of the different administrative domains. Experiments show that applications using Armada perform well in both low- and high-bandwidth environments, and that our approach does an exceptional job of hiding the network latency inherent in grid computing.