A commercial grade of zircon (ZrSiO4) concentrate was mechanically milled with MgO for up to 100 h in a laboratory-scale mill. The resultant powders were subjected to thermal processing, chemical leaching, and X-ray diffraction (XRD). There was no direct evidence of reaction during the milling step, with no new phases evident from XRD. Leaching of the powder showed that a reaction had occurred, and increased solubility with milling time was attributed to the formation of a nanostructured Mg-Zr-Si oxide, which dissolved congruently. Heating the powders resulted in a number of thermal events, including the formation/crystallization of ZrO2 and Mg2SiO4. Thermal treatment of the milled powders allowed selective chemical leaching of the magnesium, and silicon, leaving a powder containing similar to90% ZrO2.