A facile sol-gel method was adopted to synthesize iron(II,III) oxide/zinc oxide/copper(II) oxide (Fe3O4/ZnO/CuO) nanocomposites with various CuO loadings at a low temperature. The prepared nanocomposites were characterized by X-ray diffraction, field-emission scanning electron microscopy, transmission electron microscopy, energy-dispersive X-ray spectroscopy, UV–Vis spectroscopy, vibrating sample magnetometry, and Brunauer-Emmett-Teller (BET) surface area analyses. The photosonocatalytic properties of the nanocomposites were tested by methylene blue removal in aqueous solutions under the combination of UV or visible light and ultrasound. The catalyst with the lowest CuO loading exhibited the highest photosonocatalytic performance under UV light, while the fastest degradation under visible light was achieved at the highest CuO loading. Overall, the photosonocatalytic process with light and ultrasound irradiation led to more complete degradation compared to using light alone. According to the experiments performed with radical scavengers, the holes and OH radicals are the dominant oxidative species. The nanocomposites can be easily separated from the treated solution using an external magnetic field, and the samples remain very stable after 4 cycles. These results indicate that these materials have great potential for treating organic pollutants in wastewaters.