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This report summarizes the discussions from a workshop convened at NSF on May 30-31, 2018 in Alexandria, VA. The overarching objective of the workshop was to rethink the nature and composition of the NSF-supported computational ecosystem given changing application requirements and resources and technology landscapes. The workshop included roughly 50 participants, drawn from high-performance computing (HPC) centers, campus computing facilities, cloud service providers (academic and commercial), and distributed resource providers. Participants spanned both large research institutions and smaller universities. Organized by Daniel Reed (University of Utah, chair), David Lifka (Cornell University), David Swanson (University of Nebraska), Rommie Amaro (UCSD), and Nancy Wilkins-Diehr (UCSD/SDSC), the workshop was motivated by the following observations. First, there have been dramatic changes in the number and nature of applications using NSF-funded resources, as well as their resource needs. As a result, there are new demands on the type (e.g., data centric) and location (e.g., close to the data or the users) of the resources as well as new usage modes (e.g., on-demand and elastic). Second, there have been dramatic changes in the landscape of technologies, resources, and delivery mechanisms, spanning large scientific instruments, ubiquitous sensors, and cloud services, among others.