An ultrasound-assisted method was used to prepare gadolinium oxide (Gd2O3)-zeolitic imidazolate framework (ZIF)-8 nanocomposites. The surface morphology, particle size, and properties of the Gd2O3-ZIF-8 nanocomposites were examined using scanning electron microscopy (SEM), X-ray diffraction (XRD), Raman spectroscopy, and ultraviolet-visible (UV-vis) spectroscopy. The synthesized Gd2O3-ZIF-8 nanocomposites were used as a catalyst to degrade methyl orange (MO) under UV light irradiation at 254 nm. The color of the aqueous MO dye solution during photocatalytic degradation was examined using color spectroscopy. Response surface methodology (RSM) using a four-factor Box-Behnken design (BBD) was used to design the experiments and optimize the photocatalytic degradation of MO. The significance of the experimental factors and their interactions were determined using analysis of variance (ANOVA). The efficiency of Gd2O3-ZIF-8 nanocomposites for the photocatalytic degradation of MO reached 98.05% within 40 min under UV irradiation at 254 nm under the experimental conditions of pH 3.3, 0.4 g/L catalyst dose, 0.0630 mM MO concentration, and 431.79 mg/L H2O2 concentration. The kinetics study showed that the MO photocatalytic degradation followed a pseudo-first-order reaction rate law.