We investigate the effect of atomic ordering on the magnetic anisotropy of Ni80Fe20 at.% (Py). To this end, Py films were grown epitaxially on MgO (001) using dc magnetron sputtering (dcMS) and high power impulse magnetron sputtering (HiPIMS)... Aside from twin boundaries observed in the latter case, both methods present high quality single crystals with cube-on-cube epitaxial relationship as verified by the polar mapping of important crystal planes. However, X-ray diffraction results indicate higher order for the dcMS deposited film towards L12 Ni3Fe superlattice. This difference can be understood by the very high deposition rate of HiPIMS during each pulse which suppresses adatom mobility and ordering. We show that the dcMS deposited film presents biaxial anisotropy while HiPIMS deposition gives well defined uniaxial anisotropy. Thus, higher order achieved in the dcMS deposition behaves as predicted by magnetocrystalline anisotropy i.e. easy axis along the [111] direction that forced in the plane along the [110] direction due to shape anisotropy. The uniaxial behaviour in HiPIMS deposited film then can be explained by pair ordering or more recent localized composition non-uniformity theories. Further, we studied magnetoresistance of the films along the [100] directions using an extended van der Pauw method. We find that the electrical resistivities of the dcMS deposited film are lower than in their HiPIMS counterparts verifying the higher order in the dcMS case. (read more)