During Phase I of the HTMDEC program, the BIRDSHOT team focused on demonstrating the capability to execute each of the HTMDEC major capability thrusts (high-throughput synthesis, characterization, testing, simulation) in an integrated manner within a principled iterative Bayesian Optimization (BO) framework. We aimed to explore the CoCrFeNiVAl FCC HEA space to optimally find the Pareto front comprising three major performance objectives: ultimate strength/yield strength ratio, hardness, and strain rate sensitivity. The objective was to identify the Pareto optimal set over this three-objective space in at least four iterative loops. Using VAM as the main synthesis route, we demonstrated five iterative synthesis-characterization-testing-design loops involving complex protocols that include tensile experiments, high strain rate nanoindentation, spherical indentation, and LIPIT. Moreover, we have created and deployed a highly integrated cyber-physical workflow that includes the design of tailored information management protocols, accounting for each sample’s provenance and all the synthesis, processing, and characterization tasks necessary to carry out our optimal exploration. We have also developed and demonstrated an approach to connect mechanical tests to AI/ML-assisted physics-based simulations of high strain rate response. Using a state-of-the-art Bayesian Optimization framework, we have discovered, for the first time, the 3-objective Pareto set in this alloy space, exploring just 0.15% of the available feasible space.