Agúndez and coworkers reported an initial, tentative detection of silyl cyanide (SiH₃CN) in 2014, along with the confimation of C₅S and a couple other tentative detections. Three weak features observed toward IRC +10216 with the IRAM 30m telescope were assigned to SiH₃CN. Subsequent work by Cernicharo et al reported in 2017 analyzed 30 years of IRAM data. This led to better resolution of the three original rotational transitions reported in 2014 and the addition of three more lines. The presence of SiH₃CN toward IRC +10216 was thus confirmed.

Silyl cyanide is not known in terrestrial chemistry beyond studies where it has been generated in the lab, such as work by Priem et al. and by Blair et al. The cyano/cyanide family is easily the largest collection of observed astromolecules with a common group, with at least 35 compounds detected to date in the ISM/CSM.