In this research, Fe3O4 nanoparticles were synthesized via a simple co-precipitation method. Subsequently, these nanoparticles were used to synthesize TiO2-Fe3O4 nanocomposites via solvothermal ultrasonic-assisted method. Obtained nanomaterials Fe3O4 and TiO2-Fe3O4 were structurally characterized by UV–visible, XRD, and SEM-EDS. Synthesized nano-catalysts were tested as catalysis of organic dye degradation. Furthermore, an optimization study was conducted to evaluate selected TiO2-Fe3O4 nanocomposites to degrade Methylene Blue (MB) in an aqueous solution through Fenton-like reactions. Several experimental variables, including pH (from 2 to 8), H2O2 concentration (from 10-2 to 5.10-1M), catalyst amount (20 to 80 mg), and target organic compound concentrations, were tested in order to optimize the Fenton-like catalytic activity of the TiO2-Fe3O4 as a nano-catalyst to degrading MB under ambient light conditions (natural sunlight). The results showed that TiO2-Fe3O4 had an efficient degradation rate of up to 85% for MB at the optimal pH 3, H2O2 at 10-1M and 40 mg/L catalyst amount. Also, the results showed the good reusability of TiO2-Fe3O4 as a nanophotocatalyst. Also, based on the results of the scavenging agent experiments, hydroxyl radicals and superoxide radicals play an important role in methylene blue (MB) photodegradation. Finally, a possible mechanism for the photocatalytic degradation of MB was proposed. In this study, the synthesis and application of TiO2-Fe3O4 nanocomposite as a nano-catalyst in the Fenton-like oxidation process demonstrated a promising eco-friendly method for treating organic pollutants in water.