Understanding the martensitic microstructure in nickel-titanium (NiTi) thin films helps to optimize their properties for applications in microsystems. Epitaxial and single-crystalline films can serve as model systems to understand the microstructure, as well as to exploit the anisotropic mechanical properties of NiTi. Here, we analyze the growth of NiTi on single-crystalline MgO(100) and Al₂O₃(0001) substrates and optimize film and buffer deposition conditions to achieve epitaxial films in (100)- and (111)-orientation. On MgO(100), we compare the transformation behavior and crystal quality of (100)-oriented NiTi films on different buffer layers. We demonstrate that a vanadium buffer layer helps to decrease the low-angle grain boundary density in the NiTi film, which inhibits undesired growth twins and leads to higher transformation temperatures. On Al₂O₃(0001), we analyze the orientation of a chromium buffer layer and find that it grows (111)-oriented only in a narrow temperature range around 500 ^∘C. By depositing the Cr buffer below the NiTi film, we can prepare (111)-oriented, epitaxial films with transformation temperatures above room temperature. Transmission electron microscopy confirms a martensitic microstructure with Guinier Preston-zone precipitates at room temperature. We identify the deposition conditions to approach the ideal single crystalline state, which is beneficial for the analysis of the martensitic microstructure and anisotropic mechanical properties in different film orientations.