X-ray powder and electron single-crystal diffraction of crystals of Li 2 TiOSiO 4 and Li 2 TiOGeO 4 showed them to be tetragonal, space group P4/nmm unit-cell parameters a 6X4379 2, c 4X40032 2 A Ê for Li 2 TiOSiO 4 and a 6X6110 8, c 4X4372 6 A Ê for Li 2 TiGeO 4 . The compounds are isostructural with their sodium analogues but are considerably compressed along the c axis owing to the smaller size of lithium compared with sodium atoms. Square-pyramidal TiO 5 groups are joined in these compounds by tetrahedral SiO 4 and GeO 4 groups, respectively. 17 O nuclear magnetic resonance spectra of the two compounds, isotopically enriched with 17 O, showed peaks due to the apical titanyl, TiÐO, and basal, bridging, TiÐOÐSi or TiÐOÐGe, oxygen atoms of the title compounds. By comparison with reference spectra, oxygen K edges and titanium L 2,3 edges of electron energy-loss spectra were tentatively assigned.