| Summary: | New small acceptor–donor (A–D) molecules have been recently investigated as a component of organic solar cells. In this research, 2-((4-(2-ethylhexyl)-1,2,3,3<i>a</i>,4,8<i>b</i>-hexahydrocyclopenta[<i>b</i>]indol-7-yl)methylene)malononitrile was prepared from 4-(2-ethylhexyl)-1,2,3,3<i>a</i>,4,8<i>b</i>-hexahydrocyclopenta[<i>b</i>]indole in a two-step process via Vilsmeier–Haack formylation and Knoevenagel reaction with malononitrile. The structures of newly synthesized compounds were established by means of elemental analysis, high-resolution mass spectrometry, <sup>1</sup>H, <sup>13</sup>C NMR, IR and UV–Vis spectroscopy, as well as mass spectrometry.
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