Lu2O3 doped with Eu3+ has been established as an excellent scintillator material for numerous applications such as lasers, optical lenses, and radiography. The material is typically manufactured via hot pressing. This process, apart from being prohibitively expensive, can also introduce major structural defects because it requires grinding/polishing to achieve high transparency and spatial resolution. To overcome these process limitations that have restricted the commercial viability of Lu2O3:Eu3+ scintillators, a technique to deposit thin films (1–10 μm) of Lu2O3:Eu3+ has been developed. This investigation characterized the growth of such thin films by radio frequency (RF) magnetron sputtering on single-crystal cubic yttria doped zirconia (YSZ) substrates. At a deposition rate of 3.3 A/s, the effects of substrate heating and orientation on coating structure property and the resultant effect on performance were evaluated. Additionally, the effect of deposition parameters and growth conditions on the radioluminescence of the coatings, excited by x-rays, was systematically examined.