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Crystals of LiCs2[N(CN)2]3 were obtained from the reaction of stoichiometric amounts of aqueous solutions of LiCl and CsBr with Ag[N(CN)2]. X-ray single-crystal structure analysis showed that LiCs2[N(CN)2]3 crystallizes isotypically to NaCs2[N(CN)2]3 and adopts the hexagonal space group P63/m (No. 176), with a = 6.8480(8), c = 14.1665(17) Å, and Z = 2. The IR and Raman spectra of the title compound exhibit modes typical for the dicyanamide anion.