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Synthesis and Crystal Structure of Cs2
U2
(P2
Se9
)(Se2
)2

Black single crystals of Cs2U2(P2Se9)(Se2)2 were synthesized at 1023 K by a solid‐state reaction. Its structure was determined by single‐crystal X‐ray diffraction methods. The compound is isostructural with Rb2U2(P2Se9)(Se2)2 and Cs2Th2(P2Se9)(Se2)2 compounds, and crystallizes in the orthorhombic space group Pbca. Cs2U2(P2Se9)(Se2)2 displays a three‐dimensional structure comprising USe9 polyhedra connected via the Se22– and P2Se9 species with channels filled by Cs atoms. From electronic structure calculations the compound is found to be a metal with a ferromagnetic arrangement of the magnetic moments.