AbstractIn this paper, molecular beam epitaxial growth of Ni2MnGa single crystal layers on GaAs (001) using a NiGa interlayer is reported. X-ray diffraction and transmission electron microscopy confirmed an epitaxial relationship of Ni2MnGa [100]“010] // GaAs [100] [010] and a tetragonal structure of the film (a = b = 5.79 Å, c = 6.07 Å). Magnetic measurements using vibrating sample and superconducting quantum interference device magnetometers revealed an in-plane magnetization of ∼200 emu/cm3at room temperature and a Curie temperature of ∼350 K. The martensitic phase transformation was observed to occur at ∼250 K