The thin films of c-plane dominated hexagonal ζ- phase Mn2N were successfully grown on a cubic MgO (001) substrate directly using plasma-assisted molecular beam epitaxy. The surface was comprehensively studied through experimental and theoretical approaches. Reflection high energy electron diffraction revealed two pseudo-cubic domains along [100]MgO and [110]MgO, and one hexagonal domain, which is 30° apart from the [100]MgO direction. Scanning tunneling microscopy was used to image and resolve the high quality surface, revealing a distorted hexagonal surface structure. Furthermore, atomic resolution of the hexagonal domain with a 2 × 2 reconstructed surface is presented. For the c-plane surface, theoretical investigations were carried out using first-principle studies to determine the surface formation energy for various reconstructed surfaces. The theoretical study shows that the nitrogen terminated 2 × 2 structure with a manganese adatom on the surface is the most stable reconstruction that reproduces the experimental results. A corresponding simulated scanning tunneling microscopy model is also presented, providing strong support for the experimentally observed in-plane lattice structures. The manganese:nitrogen stoichiometry within the bulk and surface is in good agreement with the expected ratio of 2:1.