Highly porous yttrium oxide is fabricated as ion beam target material in order to produce radioactive ion beams via the Isotope Separation On Line (ISOL) method. Freeze casting allows the formation of an aligned pore structure in these target materials to improve the isotope release. Aqueous suspensions containing a solid loading of 10, 15, and 20 vol% were solidified with a unidirectional freeze-casting setup. The pore size and pore structure of the yttrium oxide freeze-casts are highly affected by the amount of solid loading. The porosity ranges from 72 to 84% and the crosslinking between the aligned channels increases with increasing solid loading. Thermal aging of the final target materials shows that an operation temperature of 1400 °C for 96 h has no significant effect on the microstructure. Thermo-mechanical calculation results, based on a FLUKA simulation, are compared to measured compressive strength and forecast the mechanical integrity of the target materials during operation. Even though they were developed for the particular purpose of the production of short-lived radioactive isotopes, the yttria freeze-cast scaffolds can serve multiple other purposes, such as catalyst support frameworks or high-temperature fume filters.