The bilayer thin films of CuInSe2 (CIS) and CuGaSe2 (CGS) are fabricated by a molecular beam deposition (MBD) technique by sequential depositions of CGS followed by CIS and vise versa on Mo-coated sodalime glass (SLG) and Mo/Al2O3-coated (Na blocking) SLG substrates. The thicknesses of CIS/CGS layers are adjusted to have the overall x=[Ga]/([In] + [Ga]) at approximately 0.4 similar to what is generally used in CIGS thin film solar cells. The growth temperature and the Cu-ratio y=[Cu]/([In]+ [Ga]) of the CIS and CGS layers are systematically varied for Cu-rich (y > 1) and Cu-poor (y < 1) conditions. X-ray diffraction (XRD) technique is used to analyze the shift of diffraction peaks of the preferred orientations of the bilayers compared to those of the single-layer CIS, CGS and CIGS thin films. The XRD results show that higher Ga diffusion is observed in the Cu-rich CIS/CGS bilayer rather than others. The results suggest that the diffusion of Ga is enhanced by the excess Cu-Se phase that is dependent upon the substrate temperature. The Na from the SLG substrate is one of the important factors affecting Ga diffusion. The results show alloying CIGS patterns rather than separated CIS and CGS patterns as observed in the bilayers with Na. (C) 2015 Elsevier B.V. All rights reserved.