Configuring the parameters of additive manufacturing processes for metal alloys is a challenging problem due to complex relationships between input parameters (e.g., laser power, scan speed, and material feed rate) and quality of printed outputs. The standard trial-and-error approach to find feasible parameter configurations is highly inefficient because validating each input configuration is expensive in terms of resources (physical and human labor) and the configuration space is very large. This paper applies the general principle of AI-driven adaptive experimental design for optimization to the more challenging problem of discovering feasible configurations. The key idea is to build a probabilistic surrogate model from past experiments to intelligently select a small batch of input configurations for validation in each iteration. To demonstrate the effectiveness of this methodology, we deploy it for Directed Energy Deposition (DED) process to print GRCop-42, a high-performance copper–chromium–niobium alloy developed by NASA for extreme-temperature aerospace applications. Within weeks, our approach yielded multiple defect-free outputs across a range of laser powers—dramatically reducing time-to-result and resource expenditure compared to four months of manual experimentation by our collaborators with little to no success. By enabling high-quality GRCop-42 fabrication on readily available infrared laser platforms for the first-time, we democratize access to this critical alloy, paving the way for cost-effective, decentralized production of rocket engine chambers, heat exchangers, and other high-heat-flux components.