A uranium(VI) complex UO2(L-Sal)EtOH has been synthesized by template reaction of 2-hydroxyacetophenone S-pentyl isothiosemicarbazone.hydrogen bromide (H2L), and salicylaldehyde (Sal) in the presence of uranium acetate salt. The complex was characterized by elemental analyses, IR, mass, UV–Vis, and X-ray diffraction methods. The crystal structure of the complex shows a distorted pentagonal bipyramidal geometry, where the oxo atoms occupy the axial positions and the pentagonal plane is defined by the N2O2 atoms of the tetradentate Schiff base ligand and the O atom of the ethanol molecule. The N2O2 donor ligand is coordinated to uranium(VI) via both deprotonated phenolic oxygen and azomethine nitrogen atoms.