The integration of MoS2 on low dislocation-density bulk GaN can be strategic for the realization of “truly” vertical devices. In this paper, we report the growth of ultrathin MoS2 films, mostly composed by single-layers (1L), onto homoepitaxial n--GaN on n+ bulk substrates by sulfurization of a pre-deposited MoOx film. Highly uniform and conformal coverage of the GaN surface was demonstrated by atomic force microscopy, while very low tensile strain (~ 0.1%) and a significant p+-type doping (~ 6× 1012 cm-2) of MoS2 film was evaluated by Raman mapping. Atomic resolution structural and compositional analyses by aberration-corrected electron microscopy revealed a nearly-ideal van der Waals interface between MoS2 and the Ga-terminated GaN crystal, where only the topmost Ga atoms are affected by oxidation during the MoS2 growth process. Furthermore, the relevant lattice parameters of the MoS2/GaN heterojunction, such as the van der Waals gap, were measured with high precision. Finally, the vertical current injection across this 2D/3D heterojunction has been investigated by nanoscale current-voltage analyses performed by conductive atomic force microscopy, showing a rectifying behavior with an average turn-on voltage Von= 1.7 V under forward bias, consistent with the expected band alignment at the interface between p+ doped 1L-MoS2 and n-GaN.