Two organically templated layered uranium(VI) phosphates have been prepared under hydrothermal conditions from U3O8 and H3PO4 using either NPr4+ or NHEt3+ ions as structure directing agents; both compounds have layered structures which contain infinite chains of edge-sharing [UO7] pentagonal bipyramids cross linked by bridging [PO4] tetrahedra to form two dimensional sheets of [(UO2)n-(HPO4)n-1(PO4)] mm- anions.