As microreactors evolve to become a more affordable and efficient worldwide energy source, the development of moderator material within the system to decrease the required mass of low-enriched uranium fuel is important. The use of low- instead of high-enriched uranium in small nuclear reactors stems from recent national policies associated with nonproliferation. New designs are being developed for a range of applications and nuclear space systems in particular. Using system geometries such as those described in this paper, the next step is to advance the technology readiness level of moderator material such as delta-yttrium hydride (YHx,x = 1.6–2.0) so that it can be qualified for use in a microreactor system. Although characterization of unirradiated material has been documented previously, to fully understand the performance of this material, behavior in relevant irradiation environments must occur. This paper describes the fabrication of yttrium hydride samples through innovative techniques and how these samples were tested in two relevant neutron environments. These two experiments include (1) a critical experiment performed at the National Criticality Experiments Research Center (NCERC) to evaluate reactivity changes in a neutron-critical environment and (2) irradiation in the Advanced Test Reactor (ATR) to assess structural integrity/material form, thermophysical data, hydrogen permeability, and other features post irradiation. For this purpose, hundreds of samples were fabricated for the NCERC and ATR experiments and are described within this paper.