AbstractAccess to reliable, clean energy sources is a major concern for national security. Much research is focused on the “grand challenge” of producing energy via controlled fusion reactions in a laboratory setting. For fusion experiments, specifically inertial confinement fusion (ICF), to produce sufficient energy, the fusion reactions in the ICF fuel need to become self‐sustaining and burn deuterium‐tritium (DT) fuel efficiently. The recent record‐breaking NIF ignition shot was able to achieve this goal as well as produce more energy than used to drive the experiment. This achievement brings self‐sustaining fusion‐based power systems closer than ever before, capable of providing humans with access to secure, renewable energy. In order to further progress toward the actualization of such power systems, more ICF experiments need to be conducted at large laser facilities such as the United States's National Ignition Facility (NIF) or France's Laser Mega‐Joule. The high cost per shot and limited number of shots that are possible per year make it prohibitive to perform large numbers of experiments. As such, experimental design relies heavily on complex predictive physics simulations for high‐fidelity “preshot” analysis. These multidimensional, multi‐physics, high‐fidelity simulations have to account for a variety of input parameters as well as modeling the extreme conditions (pressures and densities) present at ignition. Such simulations (especially in 3D) can become computationally prohibitive to turn around for each ICF experiment. In this work, we explore using Bayesian optimization with Gaussian processes (GPs) to find optimal designs for ICF double shell targets, while keeping computational costs to manageable levels. These double shell targets have an inner shell that grades from beryllium on the outer surface to the higher Z material molybdenum, as opposed to the nominally used tungsten, on the inside in order to trade off between the high performance associated with high density inner shells and capsule stability. We describe our results for “capsule‐only” xRAGE simulations to study the physics between different capsule designs, inner shell materials, and potential for future experiments.