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[en] The compound Cs[OCN] has been synthesized and its crystal structure and Raman spectrum were determined on selected single crystals. As postulated in earlier work, the title compound crystallizes isopointal to KN exhibiting the space group I4/mcm (no. 140, Z = 4) with the lattice parameters a = 653.79(2) and c = 799.42(5) pm. The Raman spectrum verified the nature of the triatomic moiety and shows the frequencies typical for an [OCN] anion with Fermi resonance between the 2δ and the ν vibrations. The undisturbed frequencies and the resulting force constants have been calculated and compared to those of other alkali metal compounds containing comparable linear triatomic anions.