MgAl2O4 films have been grown epitaxially on both Si(100) and MgO(100) by a novel single source metal-organic chemical vapor deposition (MOCVD) process. A single molecular source reagent [magnesium dialuminum isopropoxide, MgAl2(OC3H7)8] having the desired Mg: Al ratio was dissolved in a liquid solution and flash-vaporized into the reactor. Both thermal and plasma-enhanced MOCVD were used to grow epitaxial MgAl2O4 thin films. The Mg: Al ratio in the deposited films was the same as that of the starting compound (Mg: Al = 1:2) over a wide range of deposition conditions. The deposition temperature required for the formation of crystalline spinel was found to be significantly reduced and crystallinity was much improved on Si by using a remote plasma-enhanced MOCVD process. The epitaxial nature of the MgAl2O4 films was established by x-ray pole figure analysis.