MTiO3 (M = Fe, Mn, Ni) compounds have received recent attention as possible candidates for multiferroic materials capable of magnetization switching by application of an electric field. In an attempt to stabilize NiTiO3 in the rhombohedral R3 structure, epitaxial Ni1-xTi1-yO3 films of different thickness and composition were deposited on Al2O3(0001) by pulsed laser deposition, and characterized using several techniques. Structural parameters for ilmenite-type NiTiO3 and the metastable LiNbO3-type NiTiO3 structure with the space group R3c were predicted using density functional theory calculations, and compared with the experimental results. Our structural data from X-ray diffraction and X-ray absorption spectroscopy indicate that epitaxial ilmenite-type NiTiO3 films were grown. Furthermore, lattice strain exerted by the sapphire substrate results in a distorted ilmenite structure similar to the LiNbO3-type one. While R3c NiTiO3, the desired structure based on recent theory, cannot be claimed at this point, our results demonstrate the potential of oxide heteroepitaxy to stabilize metastable multiferroic phases that may be difficult to prepare or are inaccessible in the bulk. Published by Elsevier B.V.