Abstract. Ga+ ion irradiation-induced changes in magnetic anisotropy of a Pt/Co/Pt ultrathin film are investigated by means of the X-ray magnetic circular dichroism (XMCD) technique. A large difference in the Co orbital moment is observed between out-of-plane and in-plane directions of the film at moderate Ga + fluences of ~1-2×10 14 ions/cm 2 , which corresponds to the perpendicular magnetic anisotropy (PMA), while further increased fluences reduce the orbital moment difference, resulting in in-plane magnetization. In contrast, at much higher Ga + fluences of ~5×10 15 ions/cm 2 , at which PMA is observed again, no significant difference is found in the orbital moment of Co between out-of-plane and in-plane directions. Different origins are thus suggested for the appearance of PMA induced by the irradiation between moderate and high Ga + fluences.