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In this work, a design strategy based on a typical multi-principal element alloy (Fe₅₀Mn₃₀Co₁₀Cr₁₀, at. %) was proposed to tune the irradiation behavior by adding interstitial carbon atoms (Fe_49.5Mn₃₀Co₁₀Cr₁₀C_0.5, at. %). Advanced scanning transmission electron microscopy was employed to study the evolution of dislocation loops and helium bubbles in alloys after 400 keV He⁺ ion irradiation at three different temperatures ranging from 350 °C to 450 °C. The results showed that the interstitial carbon atoms inhibited the growth of He bubbles and irradiation hardening. The high-resolution energy dispersive spectroscopy mapping revealed that the segregation at the dislocation loops in Fe_49.5Mn₃₀Co₁₀Cr₁₀C_0.5 was efficiently lessened compared to that in Fe₅₀Mn₃₀Co₁₀Cr₁₀, which shows an even superior performance than the equiatomic FeMnCoCrNi Cantor alloy. Radiation-induced “W-shaped …