Ion implantation and thermal processing have been used to synthesize compound semiconductor nanocrystals (SiGe, GaAs, and CdSe) in both SiO2 and (0001) Al2O3. Equal doses of each constituent are implanted sequentially at energies chosen to give an overlap of the profiles. Subsequent annealing results in precipitation and the formation of compound nanocrystals. In SiO2 substrates, nanocrystals are nearly spherical and randomly oriented. In Al2O3, nanocrystals exhibit strong orientation both in-plane and along the surface normal.