Single crystals of four new uranyl titanates have been grown via the flux growth method using mixed alkali halide fluxes. Na-2(UO2)(TiO)O-3 and KNa(UO2)(TiO)O-3 have analogous layered structures containing titanyl (TiO2) units coordinated into TiO5 square pyramids. Cs-2(UO2)TiO4 crystallizes in the Cs2USiO6 structure type and is a rare example of a structure containing TiO4 tetrahedra. Cs-2(UO2)Ti2O6 crystallizes in a new tunnel structure and contains the also rare TiO s trigonal bipyramids. DFT studies were performed to understand the bonding in the observed titanate polyhedra. Furthermore, the luminescence properties of the compounds are reported, and leaching studies are reported for Cs-2(UO2)Ti2O6.