Datasets and images of the publication "Probing crystallinity and grain structure of 2D materials and 2D-like van der Waals heterostructures by low-voltage electron diffraction" - DOI: 10.1002/pssa.202300148 The Jupyter Notebooks for analyzing the datasets and generating all the figures are available at https://gitlab.com/JohMu/tds_hios_manuscript. MoS2 4D-STEM dataset: 192x192 scan pixels 200x200 camera pixels Acceleration voltage: 20kV Camera length: 10.56 mm Camera pixel size: 4x5.86 µm = 23.44 µm (original dataset with 4x4 binning) File location: Figure 2_3_S1.zip -> 230101205338_20kV_hexz0_camz-10_posi_003_good\scan_data_bin2_centered_crop-imgNx200.h5 The original raw dataset (23 GB, 192x192 scan pixels, 800x800 camera pixels, camera pixel size: 5.86 µm), the scan reference dataset and the Jupyter Notebook for the shift-compensation is available from the author. The dataset uploaded here is binned by a factor of 4 and shift-compensated. C60/MoS2 4D-STEM dataset: 113x113 scan pixels 512x512 camera pixels Acceleration voltage: 20kV Camera length: 20.56 mm Camera pixel size: 5.86 µm File location: Figure 4.zip -> scan_data_scan113x113_gzip.h5