We report the epitaxial growth of c-plane GaN films on a novel langasite IJLa 3 Ga 5 SiO 14 , LGS) substrate by plasma-assisted molecular beam epitaxy. The in-plane epitaxial relationship and the structural properties of GaN films on an LGS substrate were investigated using in situ reflective high energy electron diffraction (RHEED), high resolution X-ray diffraction (HR-XRD) and Raman spectroscopy. The in-plane epitaxial relationship between GaN and LGS determined using RHEED pattern was found to be GaNij1010]//LGSij2130]and GaNij1120]//LGSij1450]. HR-XRD results confirmed the exact epitaxial relationship, and showed that six reflection peaks of GaNIJ1012) were shifted around 19°from those of LGSIJ1012). Raman analysis revealed that a minute compressive strain still existed in the GaN film due to the very small lattice mismatch between GaN and LGS. The results obtained in this study demonstrate that the nearly lattice-matched LGS can be a promising and futuristic substrate material for the growth of GaN, and it is foreseen that our results could be a reference for the further development of high performance nitride-based devices.