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Fe-based metallic glasses have been demonstrated as effective heterogeneous catalysts in Fenton-like processes for dye degradation. Yet, currently corresponding studies have limitations due to the limited study object (dyes) and the correlation between metallic glasses and dye pollutants in Fenton-like processes is still not comprehensively studied. Accordingly, this work intensively investigated the thermal catalytic behavior correlations between two Fe-based metallic glasses (Fe₇₈Si₉B₁₃ and Fe_73.5Si_13.5B₉Cu₁Nb₃) and eight different dyes. Results indicated a lower activation energy in the more active metallic glass and a dependence of the activation energy of Fe-based metallic glasses in dye solutions. In addition, a high H₂O₂ concentration led to a declined catalytic efficiency but a photo-enhanced Fenton-like process overcame this limitation at high concentration of H₂O₂ due to the decrease of pH and enhancement of irradiation. Furthermore, the average mineralization rates of Fe₇₈Si₉B₁₃ and Fe_73.5Si_13.5B₉Cu₁Nb₃ have been measured to be 42.7% and 12.6%, respectively, and the correlation between decolorization and mineralization revealed that a faster decolorization in a Fenton-like process contributed to a higher mineralization rate. This work provides an intrinsic viewpoint of the correlation between Fe-based metallic glasses and dyes in Fenton-like processes and holds the promise to further promote the industrial value of metallic glasses.