Transmission electron microscopy (TEM) has been used for decades to establish a fundamental understanding of crystal structure and microstructure across a broad range of (inorganic) materials. However, the beam-radiation sensitivity of organic crystals has, until recently, limited the application of conventional TEM techniques to explore the microstructure of these systems. As a result, the characterization of microstructural features such as defects in organic crystals is a relatively nascent field . Different electron diffraction acquisition modalities can overcome challenges associated with structural characterization of organic crystals, namely: (1) 3D electron diffraction (3D-ED) , and (2) 4D scanning transmission electron microscopy (4D-STEM) . Over the past decade, 3D-ED has developed as a powerful technique for structure determination of micron-sized organic crystals , and is of particular importance in instances where material is scarce, or single crystals of sufficient size for singlecrystal X-ray diffraction (SCXRD) are difficult to grow. In 3D-ED, parallel illumination, with a beam typically ca. 1 micron in diameter, is used to collect diffraction patterns. For heterogeneous regions of interest with perhaps varying domain structures, the resultant pattern will be a superposition of the diffracted signal from across those domains. By contrast, 4D-STEM uses a quasi-parallel (diffraction-limited) beam a few nm in diameter to raster-scan across a region of interest. A 2D diffraction pattern is acquired at every pixel in the 2D raster scan thus creating a crystallographically-rich 4D data set. Once acquired, diffraction patterns from sub-regions can be determined, orientational variations in those patterns plotted across regions of interest, and virtual bright-field (VBF) or virtual dark-field (VDF) images reconstructed by plotting the spatial variation of a particular diffracted intensity (chosen using a virtual objective aperture).