As anionic alloy or layered compounds, layered double hydroxides (LDH) have recently attracted muchattention due to their excellent adsorption and catalytic properties. In this work, NiFe layered doublehydroxide (NiFeLDH) was utilized as a precursor to synthesize NiFeLDH/Au nanocomposites via a simpleurea-hydrolyzed hydrothermal process under UV–vis light irradiation. The as-prepared nanomaterialswere characterized using XRD, FT-IR, XPS, BET, UV–vis, TEM, and FESEM analysis. The performance ofNiFeLDH and NiFeLDH/Au nanocomposites was evaluated in the adsorptive removal of congo red (CR)dye from aqueous media using two methods of adsorption, i.e. liquid phase sorption (MS) and sonosorption(US). The sono-sorption technique exhibited higher removal efficiency due to the generationof small bubbles, strong shock waves, high-velocity microjets, and diminished thickness of diffusion layers. Furthermore, the NiFeLDH/Au nanocomposite offered much higher performance in CR removal,exhibiting a dye removal efficiency of 95% in 7 minutes of sono-sorption time. The superior performanceof the NiFeLDH/Au composite can be assigned to the high specific surface area of the sorbent, better dispersionof Au nanoparticles onto the surface of NiFeLDH materials, and synergistic effects between Auand NiFeLDH. Also, the isothermal evaluation showed that the data of CR adsorption onto fabricatednanohybrids could be well-matched with the Langmuir model indicating uniform surface energies. Moreover, kinetics studies revealed that the best data fitting for CR adsorption can be provided byHo’s pseudo-second-order kinetics. The thermodynamic study revealed that the adsorption of CR dyeonto NiFeLDH/Au was an endothermic and spontaneous process at the investigated temperatures andCR concentrations. Finally, this research suggests a simple method for the synthesis of an LDH-basednano-sorbent capable of almost completely removing organic dyes from aqueous media.