It is known that polyhalogeno-nitro-1,3-butadienes are important starting materials for the synthesis of polyfunctionalized bioactive heterocycles. Novel N,S-substituted nitrobutadienes (4a-j) were synthesized from the reaction of the monothio-substituted nitrodiene derivatives (2a) and (2b) with some piperazine derivatives. These new compounds are stable and the structures of these products were characterized by spectroscopic data. The structure of the novel N,S-substituted nitrodiene compound (4g) synthesized in this study was also elucidated by single crystal x-ray analysis.