The data were generated using an automated workflow modified from Reference . We retrieved the crystallographic information framework (CIF) files from the Materials Project database . In these files, it was necessary to regenerate the symmetry information (i.e., space groups and symmetry operations). Using the FINDSYM software , we obtained the crystal system for each structure. We developed an electron diffraction simulator using the open-source Pymatgen package . Given an incident beam direction, the simulator generates the positions and intensities of Bragg disks, from which we can construct vector maps. We adopted the following principle for zone axis sampling. The sampling covers zone axes [u v w] in the 1/8 sphere (due to symmetry) (Fig. ), with integer u, v and w values in the range from 0 to 5 (except all zeros). For two zone axes that are close (i.e., the angle between them is below a threshold), only the lower order ones will be sampled. The threshold for training and testing data are 10° and 5°, respectively. Thus, the testing data contains DPs from zone axes unseen in the training data, which matches the scenario of applying the trained model to real experimental data. In total, there are 34 zone axes for training and 94 for testing. Training and testing sets each include 500 randomly sampled crystal structures per crystal system. For each crystal, DPs are simulated with the above zone axes. The resulting training data size is 500 × 7 × 34 = 119,000 and testing data size is 500 × 7 × 94 = 329,000.