The present work suggests that the chelate UO2(C9H6NO)2.C9H6NOH can be crystallized from chloroform as orange-red crystals which are monoclinic, space groupP21witha = 14.98 Å (σ = 0.03 Å),b = 20.38 Å (σ = 0.05 Å),c = 14.75 Å (σ = 0.03 Å), and β = 115.32° (σ = 0.20°). It is believed that six molecules are in the unit cell: three sets of molecules in the general positions (2a). The uranium positions have been established and show the higher symmetryP21/mwith four atoms in general positions and two atoms in the pseudo mirror planes. The molecular arrangement of 8-quinolinol molecules around the more general uranium atoms has been obtained from three-dimensional Fourier syntheses. This arrangement of 8-quinolinol molecules is essentially the same as found by Hall, Rae, and Waters in the adduct UO2(C9H6NO)2.C9H6NOH.CHCl3. The molecular arrangement around the two remaining uranium atoms has not been established because of false detail introduced by the pseudo-symmetry. This is enhanced by pronounced termination of series errors in theb-axis direction.