A cyclic heat-treatment process was used to prepare single grains of the quasicrystalline icosahedral phase, ψ–Al65Cu23Fe12. Alloys of appropriate composition are melted and chill cast into copper molds. Multiple cyclic heat treatments at successively higher temperatures below 860 °C, the peritectic decomposition temperature of the quasicrystal phase, are used to enhance the growth of the ψ phase. Single grains up to 10 mm × 5 mm × 5 mm have been prepared.