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Autonomous experimentation systems have been used to greatly advance the integrated computational materials engineering (ICME) paradigm. This paper outlines a framework that enables the design and selection of data collection workflows for autonomous experimentation systems. The framework first searches for data collection workflows that generate high-quality information and then selects the workflow that generates the best, highest-value information as per a userdefined objective. We employ this framework to select the user-defined best high-throughput workflow for material characterization on an additively manufactured Ti-6Al-4V sample for the purposes of outlining a basic materials characterization scenario, reducing the collection time of backscattered electron scanning electron scanning electron microscopy images by a factor of 5 times as compared to the benchmark workflow for the case study presented, and by a factor of 85 times as compared to the workflow used in the previously published study.