The bismuth ferrite/ZnMgAl-LDH (BFO/LDH) nanocomposite was successfully synthesized in the in situ co-precipitation method as an enhanced adsorbent of methylene blue dye under sonication interference. The synthetic structure was deeply characterized by different structural, chemical, textural, and physical techniques, including XRD, FT-IR, Raman analysis, BET surface area TEM, and XPS. The charterization findings describe the formation of the composite as magnetic spherical-like nanoparticles with a grain size less than 100 nm, a surface area of 13.4 m2 g–1, and multifunctional active chemical groups. The composite was applied to adsorb methylene blue (MB) via adsorption from an aqueous solution. MB adsorption experiments were conducted in an ultrasonic bath, and the effect of various adsorption parameters such as composite dosage, pH, time, and initial dye concentration has been briefly studied. The result indicated that pH 12 is more optimal for MB adsorption. The adsorption kinetics of the composite are determined to be pseudo-second-order. Furthermore, BFO/LDH composites exhibit a higher adsorption capacity (244.49 mg g−1) under optimal conditions. The equilibrium adsorption isotherm follows the Langmuir isotherm model. The results indicate that the prepared BFO/LDH composite provides a novel effective adsorbent for MB from aqueous media and could be applied for actual wastewater purification.