A　novel　D3T　derivative,　5-amino-4-cyano-3H-1,2-dithiole-3-thione　(compound　1)　has　been　obtained　in　one-pot　reaction.　The　crystal　is　orthorhombic,　space　group　Pbca,　with　a　=　10.3667(4)　Å,　b　=　10.8898(4)　Å,　c　=　11.4942(5)　Å,　V　=　1297.60(9)　Å3,　and　Z　=　8.　In　the　crystal,　molecules　are　firstly　self-assembled　into　a　complex　sheet　parallel　to　the　(0　0　1)　plane　containing　centrosymmetric　R24　(16)　and　R44　(24)　rings,　and　then　the　interconnection　of　molecular　sheets　through　S··S　interactions　forms　a　three-dimensional　supramolecular　assembly.　The　DFT　calculations　are　performed　for　isolated　molecule　using　the　B3LYP/6-31+G(d,p)　methods.　The　frontier　orbital　properties　of　compound　1　have　been　reported　and　discussed.　Moreover,　a　detailed　assignment　of　the　fundamental　vibrational　modes　is　proposed　on　the　basis　of　the　calculated　results.　©　2008　Elsevier　B.V.　All　rights　reserved.