The semiconductor TlSn 2 I 5 with a two-dimensional crystal structure and an antiperovskite topology is a promising novel detection material. The compound crystallizes in the I4/mcm space group, has an indirect band gap of 2.14 eV, and melts congruently at 314 °C. Electronic band structure calculations reveal that the most facile electron transport is along the ab layered plane. Compared to CH 3 NH 3 PbX 3 (X = Br, I), TlSn 2 I 5 features higher long-term stability, higher photon stopping power (average atomic number of 55), higher resistivity (∼10 10 Ω•cm), and robust mechanical properties. Centimeter-size TlSn 2 I 5 single crystals grown from the melt by the Bridgman method can be used to fabricate detector devices, which detect Ag Kα X-rays (22 keV), 57 Co γ-rays (122 keV), and 241 Am α-particles (5.5 MeV). The mobility-lifetime product and mobility for electrons were estimated to be 1.1 × 10 −3 cm 2 •V −1 and 94 ± 16 cm 2 •V −1 •s −1 , respectively. Unlike other halide perovskites, TlSn 2 I 5 shows no signs of ionic polarization under longterm, high-voltage bias.