Uranium has attracted sustained attention due to its high mobility and biotoxicity. Among various techniques, sorption is considered as the most effective technique to treat the U(VI)-containing wastewater. In serving for low-cost adsorbents, layered double hydroxides (LDHs) have been proved to be promising candidates. However, the interaction mechanism of U(VI) with LDHs is still unclear, although plenty of LDHs have been used in this field. Herein, we developed two novel methods to fabricate ternary LDHs (MgFeAl LDHs and NiFeAl LDHs) and applied the ternary LDHs as adsorbents to investigate their sorption performance towards U(VI). The results showed that the sorption was endothermic and followed the pseudo-second-order kinetics through the formation of inner-sphere surface complexes, and the sorption isotherms were simulated by the Langmuir model well. Furthermore, systematic spectroscopy characterization indicated that the sorption occurred on the surface sites of Mg-OH and Ni2+-OH, while the CO(3)(2-)in the gallery space also played an important role. This work highlighted the synthesis of high-efficient materials and their application in wastewater treatment.