This study reports on the magnetic hardening phenomenon of heavily helium ion-irradiated iron–chromium alloys. The alloys are important structural materials in next-generation nuclear reactors. In some cases, problems may arise when the magnetic properties of the materials change due to neutron irradiation. Therefore, it is necessary to understand the effects of irradiation on magnetism. Helium irradiation was conducted as a simulated irradiation, and the effect of cavity formation on magnetic properties was thoroughly investigated. High-quality single-crystal Fe-x%Cr (x = 0, 10, 20) films, with a thickness of 180–200 nm, were fabricated through ultra-high vacuum evaporation. Subsequently, irradiation of 19 dpa with 30 keV He+ ions was conducted at room temperature. X-ray diffraction measurements and electron microscopy observations confirmed significant lattice expansion and the formation of high-density cavities after irradiation. The magnetization curve of pure iron remained unchanged, while magnetic hardening was noticed in iron–chromium alloys. This phenomenon is believed to be due to the combined effect of cavity formation and changes in the atomic arrangement of chromium.