These amorphous carbon films were generated following the deposition protocol and methodology outlined by Caro et al., Phys. Rev. Lett. 120, 166101 (2018) and, in more detail, in Caro et al. Phys. Rev. B 102, 174201 (2020). Briefly, the structures were generated by depositing monoenergetic C atoms on a preexisting diamond (111) substrate. The interatomic potential used was the a-C GAP of Deringer and Csányi [Phys. Rev. B 95, 094203 (2017)] and the molecular dynamics simulations (MD) were carried out with QUIP's GAP implementation [http://libatoms.github.io/] using LAMMPS [https://lammps.sandia.gov/] as MD engine. The final structures of the deposition simulations at 1, 2, 3, 4, 5, 6.5, 8, 10, 20, 60 and 100eV are provided in extended XYZ format, with obvious naming convention.