This dataset contains the data used in the publication entitled "Atomic structure of solute clusters in Al-Zn-Mg alloys", published in Acta Materialia 17. December 2020. The data contained herein are: As-acquired transmission electron microscopy (TEM) images. Atom probe tomography data. All structural models used in density functional theory (DFT) calculations. Structures used for simulating scanning-TEM (STEM) images and nanobeam diffraction (NBD) patterns. The TEM images includes high angle annular dark field (HAADF) images and selected area diffraction patterns. These are given in .dm3/.dm4 files, and can be opened in e.g. the "Gatan Microscopy Suite" software. The images are also given as .tif images. The files are names after the "Figx_alloy_condition_xxx". "Figx" refers to the figure in the main article, "alloy" describes the alloy used and "condition" describes from what ageing condition. The uncorrected image series used for Fig. 6c (in the article) is included and requires the SmartAlign plugin in the Gatan Microscopy Suite to analyse the dataset. SmartAlign allows for correcting rigid and non-rigid distortions in the STEM images in order to reduce effect of specimen drift and scan noise during acquisition. The ATP data is given as a .xlsx file. The data here is the processed data after applying the maximum separation algorithm. The data here is used to produce Figs. 2b and 2c in the paper. The structures used in the DFT calculations are given here as .cif files. These are separated into "Single_clusters" and "Stacked_clusters" and named according to Tabs. 1 and 2 in the Supplementary material of the paper. The two structures used for simulating STEM-HAADF and NBD patterns are given in the folder "TEM_simulations". "Mg32Zn124D_94x94" was used for NBD and "Mg32Zn124D_X_Zn4" was used for HAADF-STEM. The stack used for Supplementary Fig. 7c is labeled "Mg32Zn124D_94x94_slab_1Allayerop.cif".