Dataset associated with the publication "Planetary Boundaries Analysis of Low-Carbon Ammonia Production Routes" by Sebastiano C. D'Angelo, Selene Cobo, Abhinandan Nabera, Antonio J. Martín, Javier Pérez-Ramírez, and Gonzalo Guillén-Gosálbez, available at https://doi.org/10.1021/acssuschemeng.1c01915. The dataset includes the numeric data required to plot all the figures embedded in the main manuscript and in the Supporting Information (SI), as well as the tables presented in the SI converted in a machine-readable format. The structure of the dataset is here elucidated sheet by sheet: LCA-Total: numerical values associated with the total share of safe operating space for all the assessed control variables of the seven planetary boundaries quantified in the study, for all the considered scenarios. The results are presented for the three different downscaling approaches considered in the study. The global warming impacts for all the scenarios, calculated with the ReCiPe 2016 methodology (hierarchist approach), are here reported, as well. LCA-Breakdown: numerical values associated with the breakdown of the environmental impacts for the selection of scenarios reported in the main manuscript, for all the assessed control variables. Economics: numerical values associated with the breakdown of the economic impacts reported in the main manuscript, for all the assessed scenarios. SI-Tables-LCI: tables reported in the SI associated with the environmental assessment of all the scenarios. SI-Tables-Economics: tables reported in the SI associated with the economic assessment of all the scenarios.