Four uranyl borates, UO2B2O4 (UBO-1), alpha-(UO2)(2)[B9O14(OH)(4)] (UBO-2), beta-(UO2)(2)[B9O14(OH)(4)] (UBO-3), and (UO2)(2)[B13O20(OH)(3)]center dot 1.25H(2)O (UBO-4), have been prepared from boric acid fluxes at 190 degrees C. UBO-3 and UBO-4 are centrosymmetric, whereas UBO-1 and UBO-2 are noncentrosymmetric (chiral and polar). These uranyl borates possess layered structures constructed from UO8 hexagonal bipyramids, BO3 triangles, and 604 tetrahedra. In the case of UBO-4, clusters of BO3 triangles link the layers together to form open slabs with a thickness of almost 2 nm. The ability of uranyl borates to use very similar layers to yield both centrosymmetric and noncentrosymmetric layers is detailed in this work.