<p>In this work, the adsorption properties of uranyl ions (UO₂) on the surfaces of two-dimensional metallic materials Sb, LDH, and NiAl-LDH/Sb are investigated using density functional theory (DFT). The computational results show that LDH/Sb has the best adsorption performance for UO₂. The electronic structure, charge transfer, and electronic localization function analyses reveal that UO₂ undergoes electronic orbital coupling with Ni and Sb of LDH/Sb and transfers the highest number of charges among the three substrates, which enables its stable adsorption. The dependence of adsorption rate on temperature was calculated, and it is concluded that the desorption temperature of uranyl ions on the surface of LDH/Sb is the highest at 570&#xa0;K. The results indicate that NiAl-LDH/Sb is a good adsorbent material for uranyl ions and, therefore, has application prospects in uranium extraction from seawater.</p>