Crystalline lanthanum aluminate (LAO) films were grown epitaxially on SrTiO 3 (001) and on Si(001) with a buffer layer of four unit cells of SrTiO 3 by atomic layer deposition. The SrTiO 3 buffer layer was grown by molecular beam epitaxy. Tris(N,N'-diisopropylformamidinate)-lanthanum, trimethylaluminum, and water as co-reactants were employed at 250 °C for atomic layer deposition. Films were characterized using ex-situ reflection high-energy electron diffraction, X-ray diffraction and in-situ X-ray photoelectron spectroscopy. The as-deposited LAO films were amorphous. Different annealing conditions were necessary to realize crystalline films because of different degrees of tensile strain between crystalline LAO and the SrTiO 3 or the Si(001) substrate. When grown on SrTiO 3 (001), with a lattice mismatch of 2.9%, annealing temperatures of 750 °C for 2 h were necessary. Crystalline films were realized at 600 °C under vacuum at 2 h for SrTiO 3 -buffered Si(001), with a lattice mismatch of 1.3%. By keeping the annealing temperature relatively low (2 h at 600 °C under vacuum), the interfacial amorphous layer at the STO/Si interface was minimized to about one monolayer and an abrupt interface between SrTiO 3 and LAO was maintained.