The preparation of Se(CN)(4) was attempted by the reaction of SeF4 with Me3SiCN at low temperatures. However, selenium tetracyanide could not be detected by NMR spectroscopy; instead, the decomposition product Se(CN)(2) was isolated and its crystal structure was redetermined. In the structure of Se(CN)(2), layers are present with secondary Se center dot center dot center dot N interactions. The structure of Se(CN)(4) and its reductive decomposition reaction has been calculated at the MP2 level of theory.