The presence of methylcyanodiacetylene (CH₃C₅N) toward TMC-1 was confirmed in 2006 by Snyder et al., completing an effort that had begun more than 20 years previously. In 1984, Snyder and a mostly different team of colleagues had reported tentative evidence for the detection toward TMC-1. The initial observations were made with the Effelsberg 100m Radio Telescope in Bad Münstereifel, while the confirming observations were made with the slightly larger Green Bank 100m telescope in West Virgina.

New experimental data for methylcyanodiacetylene were reported in 2016 for its infrared/Raman and electronic spectra.

Methylcyanodiacetylene is one of at least three dozen cyano/cyanide species that have been detected to date.