Iron films produced using an arc plasma gun were studied by Mössbauer spectroscopy, and their surface features were examined using atomic force microscopy and scanning electron microscopy. The surface morphology of the iron films reflected the morphology of the substrates. When an aluminum foil with 100-nm grooves was employed as the substrate, the surface of the iron film also had grooves. The nuclear spin orientation of the iron tends to be linear along the grooves. The effects of deposition conditions on nuclear spin orientation, including the groove size on the aluminum substrates, the iron film thickness, and the temperature during deposition, were studied.