Uranium is considered to be a strategic means for the nuclear power as well as a worldwide highly toxic pollutant. For the enhanced U(VI) elimination from wastewater, novel Co-Mo-Ni ternary hydroxide (CMN) and calcined CMN (CCMN) nanocomposites were prepared via a simplistic single-step hydrothermal technique and calcination process. The elimination process and adsorption property of U(VI) on CMN and CCMN were analysed by batch experiment as well as spectroscopy analysis, and the researches showed that U(VI) was formed stable and strong complexes with the surface groups of CMN and CCMN. The maximal removal capacities of U(VI) on CMN and CCMN amounted to be 585.6 and 973.7 mg/g at pH = 5.0 and T = 298 K, correspondingly, that exhibited competitiveness with the majority of the reported adsorbents. The U(VI) uptake was substantially impacted by the tested solution pH and not affected by the ionic strength, which revealed that the interaction mechanism was primarily inner-sphere surface complexation, which received further confirmation by the XPS analysis. Based on the above analyses, the facile synthesis process and excellent U(VI) elimination performance denoted that the ternary (hydr)oxide materials were applicable as an attractive adsorbent for the radionuclides preconcentration and removal from aqueous solutions in natural environmental management.