Dataset for Neural Network training and testing of paper entitled "Machine-learning-aided atomic structure identification of interfacial ionic hydrates from AFM images" (https://doi.org/10.1093/nsr/nwac282). Each file contains named-dependent simulated AFM Images at different tip height and corresponding atomic structure file in POSCAR format. (See detailed description in the manuscript https://doi.org/10.1093/nsr/nwac282)