Five compounds of the MAn(2)Q(5) family, namely, SrU2S5, BaU2Se5, PbU2S5, BaTh2S5, and BaU2Te5, have been synthesized by high-temperature solid-state reactions. The crystal structures of these compounds were determined by single-crystal X-ray diffraction studies. SrU2S5, BaU2Se5, PbU2S5, and BaTh2S5 crystallize in the PbU2Se5 structure type in space group C(2)h(5)P(21)/c of the monoclinic system, whereas BaU2Te5 adopts the (NH4)Pb2Br5 structure type in space group D(4)h(18)I(4/mcm) of the tetragonal system. There are no QQ bonds in these structures, so the formulas charge balance as M2+(An(2)(4+)Q(5)(2). The An atoms in the monoclinic structure are seven- or eight-coordinated by Q atoms; the U atoms in the tetragonal structure are eight-coordinated. The M atoms in the monoclinic structure are coordinated to either eight or nine Q atoms, depending on the monoclinic beta angle; the M atoms in the tetragonal structure are 10-coordinated. Resistivity studies on single crystals of SrU2S5, BaU2Se5, and PbU2S5 show metallic behavior with resistivities of 0.24, 10, and 3.3 mO.cm, respectively, at 298 K. Spin-polarized density functional theory in the generalized gradient approximation applied to the four U compounds suggests that they are ferromagnetic. In each compound, the density of states of one spin channel is found to be finite at the Fermi level, whereas there is a gap in the density of states of the other spin channel; this is characteristic of a half-metal.