Dataset for Quantitative description of metal center organization in single-atom catalysts by by K. Rossi, A. Ruiz-Ferrando, D. Faust Akl, V. Gimenez Abalos, J. Heras-Domingo, R. Graux, X. Hai, J. Lu, D. Garcia-Gasulla, N. López, J. Pérez-Ramírez, and S. Mitchell. The data is structured as follows: 01_Micrographs: all micrographs employed in .tif and .png format. An imageJ macro to overlay coordinate files with images is attached. 02_Ground_truth: contains the manually-labeled and predicted xy-coordinates of atomic positions including probabilities. 03_All_detection_data: contains all automated predictions of atomic positions in the images of this study (uhd), and of Mitchell et. al in JACS, 144, 8018-8029 (2022) (jacs_train, jacs_test). This folder further contains model weights and area segmentations needed to estimate the surface atomic densities. 04_Trimetallic_analysis: Figures complementing Supplementary Figure S21.