A remote plasma enhanced-metal organic chemical vapor deposition (RPE-MOCVD) process was developed for the preparation of non-crystalline (ZrO2)x-(SiO2)1−x (x ≤ 0.5) alloys, targeting the compound composition ZrSiO4with k ∼ 12.5. Shifts in Si LVV and Zr LMM AES energies with respect to elemental values showed that the deposited film was a fully-oxidized zirconium/silicon alloy. FTIR results were consistent with AES, and a Zr-O-Si bonding mode was identified in the spectra. The films were amorphous before and after RTA at 900°C for 30 sec, as monitored via RHEED. Optical absorption measurements indicated the onset of band-to-band transitions at an energy of approximately 6 eV. Finally, C-V testing showed that the films were insulating.