Al/Al2O3 coating with a total thickness of approximately 3 μm was irradiated by 6 MeV Au-ions with the damage level from 13 to 39 dpa at room temperature. The results showed that the surface roughness of the Al/Al2O3 coating decreased with increasing irradiation damage levels. As the irradiation damage level is up to 39 dpa, the crystallinity of the Al2O3 layer is enhanced, and the irradiation-induced defects such as voids and dislocations appeared in the Al/Al2O3 coating. The decreased hardness and the deterioration of deuterium permeation resistance are strongly associated with the changed microstructure. The underlying mechanism for the evolution of microstructure and properties induced by Au-ions irradiation is discussed.