Structural quality of LuFeO 3 epitaxial layers grown by pulsed-laser deposition on sapphire substrates with and without platinum Pt interlayers has been investigated by in situ high-resolution X-ray diffraction (reciprocal-space mapping). The parameters of the structure such as size and misorientation of mosaic blocks have been determined as functions of the thickness of LuFeO 3 during growth and for different thicknesses of platinum interlayers up to 40 nm. By means of fitting of the time-resolved X-ray reflectivity curves and by in situ X-ray diffraction measurement, we demonstrate that the LuFeO 3 growth rate as well as the out-of-plane lattice parameter are almost independent from Pt interlayer thickness, while the in-plane LuFeO 3 lattice parameter decreases. We reveal that, despite the different morphologies of the Pt interlayers with different thickness, LuFeO 3 was growing as a continuous mosaic layer and the misorientation of the mosaic blocks decreases with increasing Pt thickness. The X-ray diffraction results combined with ex situ scanning electron microscopy and high-resolution transmission electron microscopy demonstrate that the Pt interlayer significantly improves the structure of LuFeO 3 by reducing the misfit of the LuFeO 3 lattice with respect to the material underneath.the hexagonal phase depend strongly on the mutual orientation of the layer and substrate lattices (epitaxial orientation) as well as on the epitaxial strain (misfit). The epitaxial orientation is determined by the minimum free energy, which is related to the bonding across the substrate-epilayer interface and to the mismatch of the substrate and layer lattices. It is recognized that, despite the triangular symmetry matching on the abovementioned substrates, there is no obvious lattice match between h-RFeO 3 and Al 2 O 3 (0001) (a = 4.7602 Å), yttrium-stabilized zirconia (YSZ) (111) (a = 7.30 Å), or Pt (111) (a = 5.548 Å) [10].Nevertheless, an epitaxial growth of h-LuFeO 3 (LFO) could be obtained using the pulsed-laser deposition [6][7][8][9]11]. This means that the azimuthal epitaxial orientation of h-LuFeO 3 films cannot be explained simply by the lattice mismatch. One should understand the interfacial structure in detail by means of structural investigations performed in situ during pulsed-laser deposition (PLD). This approach reveals how the structural setup of the layer/substrate interface would affect the structure and the morphology of the deposited h-LuFeO 3 .Epitaxial strain is an extremely important issue in epitaxial thin film growth because the strain may change the properties of the epilayer, offering opportunities of material engineering; see the reviews in References [12,13], among others. For the Al 2 O 3 (0001) substrates, the lattice mismatch of the supercell is small but the huge misfit of the lattice constant suggests weak interfacial bonding [10]. The growth of an additional Pt interlayer aims on the one side to reduce the lattice mismatch between the deposited h-LuFeO 3 layer and Al 2 O 3 (0001) substrate an...