ABSTRACTAlthough heteroepitaxy of lattice-matched and lattice-mismatched materials leading to artificially structured materials has resulted in impressive performance in various electronics devices, material combinations are usually limited by lattice matching constraints. A new concept for fabricating material systems using the atomically abrupt and low dimensional nature of layered materials, called van der Waals epitaxy (VDWE), has been developed. GaSe (Eg = 2.1 eV) has been deposited on the three dimensional surface of GaAs (111) using a molecular beam deposition system. GaSe was evaporated from a single Knudsen source, impinging on a heated substrate. Even with a lattice mismatch of 6% between the substrate and the growing film, good quality single crystal films were grown as determined by RHEED. The films have further been analyzed using a complementary combination of XPS and X-ray reflectivity.