The realm of Earth science (ES) is increasingly data-intensive. Geoinformatics research attempts to robustly smooth and accelerate the flow of data to information, information to knowledge, and knowledge to decisions and to supply necessary infrastructure and tools for advancing ES. Enabling easy access to and use of large volumes of ES data and massive computing resources is an essential role of geoinformatics for supporting ES research and education but remains a problem. There are still many challenges in solving this problem for geoinformatics. The key challenge is that the current data and information systems are not easily interoperable at the data, functions (services), and systems levels. Recent advances in cyberinfrastructure (CI), Web services, and geospatial interoperability technologies promise to overcome this challenge. This dissertation research aims at solving this problem by taking the advantage of those recent advances. Driven by the common needs of data-intensive research and education in Earth sciences, this research studies the feasibility and methodology of facilitating ES research and education with interoperable geospatial Web services, develops a service-oriented architecture (SOA) for an open, interoperable geospatial Web service system, and implements the system in an operational environment. The research also analyzes the impact of such a system on ES research and education. An integrated perspective for the common needs of ES research and education is achieved by identifying major barriers in ES research and education and the associated challenges for geoinformatics to provide solutions. The state of the art in geoinformatics for addressing those challenges is reviewed. The integrated system framework, interoperability mechanisms, functional requirements, and the methodology for building an operational geospatial Web service system are explored, with the goal of providing better data and processing services to ES research and education. The system is designed as an open, interoperable, standards-compliant, adaptable (self-evolvable and maintainable), and SOA-based geospatial Web service system. The functional requirements, as well as design principles including the system interoperability, scalability, reusability, and adaptability, have been considered comprehensively in the design of the system architecture. The implementation issues, such as the effectiveness and efficiency of the system, are explored and the strategy for dealing with these issues is discussed. The system designed is implemented and operated as GeoBrain by the NASA EOS Higher Education Alliance (NEHEA). It provides operational online on-demand ES data and processing services to worldwide users. The operational use of GeoBrain in ES research and education has demonstrated that this dissertation research has successfully solved the problem at which it aimed. The research also provides insights, lessons-learned, and technology readiness for developing more capable geospatial Web service systems for establishing more effective online learning and research environments for Earth science in the near future. Such systems can meet wide-range needs of future generations of scientists, researchers, educators and students in their formal or informal educational training, research projects, career development, and lifelong learning. [The dissertation citations contained here are published with the permission of ProQuest LLC. Further reproduction is prohibited without permission. Copies of dissertations may be obtained by Telephone (800) 1-800-521-0600. Web page: http://www.proquest.com/en-US/products/dissertations/individuals.shtml.]