4D Scanning nano-beam diffraction dataset in the NETCDF dataformat.The datasets are used in the publication: O. Maßmeyer, J. Belz, B. O. Dogahe, M. Widemann, R. Günkel, J. Glowatzki, M. Bergmann, S. Pasko, S. Krotkus, M. Heuken, A. Beyer, K. Volz, A Small Step for Epitaxy, a Large Step Toward Twist Angle Control in 2D Heterostructures. Adv. Mater. Interfaces 2024. The paper discusses the investigation of 2D heterostructures of WS2 and graphene grown by metal organic chemical vapor deposition (MOCVD) with high resolution scanning transmission electron microscopy. The datasets contain the 4D scanning nanobeam diffraction data of two different sample regions containing a monolayer and a bilayer region of WS2 on top of the graphene layers. A more detailed description of the dataset structure can be found in the attached markdown file and in the supporting information of the research article.