This dataset contains AMS-BAND electronic structures and pEDA+NOCV data (PBE+D3(BJ) / TZ2P / small frozen cores on all but Cl / ZORA / Gamma-point ) of H2O adsorptions onto a (2×2×4) unit cell large YF3 supercell (= Y64F184) of (101) orientation. The bare surface is also included. Each structure is its own .tar named according to surface + (number of) adsorbate molecules + structural isomer letter + structure number. Each structure contains the input file (.run), output file (.out) and the ams.results folder containing the log file (ams.log) and the binary AMS-BAND results files (ams.rkf, band.rkf). If the NOCV deformation density isosurface files (.vtk) were calculated, these are also included within the ams.results folder. The generation and relaxation of the atomic structures is described in: https://doi.org/10.3390/cryst13040555