Mechanofusion is an alternative fabrication technique that has the potential to advance cermet TPBAR pellets by producing LiAlO2-Zr core-shell powders that will provide tighter control of targeted microstructural characteristics such as the presence and thickness of Zr surrounding every LiAlO2 particle in the cermet. Significantly enhanced microstructural control will translate to improved control of material properties and characteristics that affect the in-reactor performance of cermet TPBAR pellets. It was the intention of this work to demonstrate the efficacy of mechanofusion for producing precursor powders for TPBAR pellets, however materials procurement issues prevented this objective from being fully realized. In spite of these issues, in the short amount of time during which appropriate materials were available, it was demonstrated that mechanofusion does indeed have promise for producing the desired structures although the process yet requires optimization.