In this work, an efficient single-step green synthesis protocol of 2,3,4,4a-tetrahydroisoquinoline-5,7-dicarbonitriles was applied with the purpose of their biological activity studies. It was found that the cytotoxic activities of 2,3,4,4a-tetrahydroisoquinoline-5,7-dicarbonitriles in the SHSY-5Y cancer cell line were most active after 72 h of incubation. It was determined that 1,6-diamino-4a-