Iron and its binary oxides are meticulously exploited for environmental remediations. However, only limited studies have been carried out on the degradation of industrial organics by advanced oxidation process. In this study, iron oxide, cobalt oxide, and iron-cobalt binary oxides were synthesized by a modified hydrothermal method as heterogeneous Fenton-like catalysts for the removal of methylene blue (MB) from wastewaters. The oxide nanostructures were characterized by different analytical techniques. Studying the effects of various parameters such as catalyst dose, MB concentration, and H 2 O 2 concentration, the reaction conditions were optimized to enhance the removal of MB dye. The results revealed that α-Fe 2 O 3-Co 3 O 4 shows much higher activity than both Co 3 O 4 and α-Fe 2 O 3 for the degradation of MB at room temperature and beyond. The binary α-Fe 2 O 3-Co 3 O 4 shows degradation efficiency of 96.4% at 65 C within 60 min. Furthermore, the binary α-Fe 2 O 3-Co 3 O 4 catalyst retains its activity for up to four successive cycles. A probable mechanism is also proposed, involving the generation of ‧OH radical as well as Fe 2+ /Fe 3+ or Co 2+ /Co 3+ redox couple of the binary α-Fe 2 O 3-Co 3 O 4 catalyst. K E Y W O R D S advanced oxidation process, catalyst, degradation, methylene blue, α-Fe 2 O 3-Co 3 O 4