Neodymium-doped zirconolite materials may be synthesized by two melting processes. One involves devitrification of an aluminosilicate parent glass containing titanium, zirconium and neodymium oxides, yielding a glass ceramic comprised of submicron zirconolite needles embedded in a silica-rich glass matrix. The second method consists of melting an oxide mixture with the stoichiometry of a highly Nd-enriched zirconolite, then quickly cooling the melt to produce a ceramic rich in zirconolite crystals several hundred microns long containing a large fraction of the initial neodymium.