Using a microwave-assisted ball-milling approach, Fe-based metal-organic frameworks (Fe-MOFs) were prepared from FeSO4·7H2O and trimesic acid. Scanning electron microscopy, Fourier-transform infrared spectrometry, X-ray, and thermogravimetric analysis were utilized to characterize the thermal stability and structure of the prepared Fe-MOFs. These Fe-MOFs were used to remove organic dyes from aqueous solutions. Specifically, they removed 96.97% of 23.3592 mg/L of Congo red in a 200 mL solution within 300 min of treatment with natural light at 15 °C. Likewise, 88.21 and 70.90% of 22.7527 mg/L of Orange II and 17.8326 mg/L of Rhodamine B, respectively, were removed from 200 mL solutions within 300 min of treatment at 15 °C. At 35 °C, 99.57, 95.98, and 99.38% of 23.3855 mg/L of Congo Red, 22.7365 mg/L of Orange II, and 17.9973 mg/L of Rhodamine B, respectively, were removed from 200 mL solutions within 300 min of treatment. The adsorption kinetics were investigated and the pseudo-first-order kinetic model was found to be superior to the pseudo-second-order kinetic model. Overall, using metal-organic frameworks to treat dye wastewater was found to be inexpensive, feasible, and efficient. Therefore, this material has future prospects in research and applications in the purification of wastewater.