Aluminum isocyanide (AlNC) was observed in the circumstellar envelope of IRC+10216 and reported in 2002 by Ziurys et al. with the IRAM 30 m telescope at Pico Veleta, Spain. The detection was made possible by experimental measurements of the spectra of AlNC by Robinson et al.,, which in turn was guided by quantum chemical predictions made by Ma et al. Both theory and experiment find that AlNC is more stable than AlCN.

Other observed isocyano species include HNC, MgNC, HMgNC, SiNC, isocyanoacetylene (HCCNC), and methyl isocyanide (CH₃NC).

Metal cyanide and isocyanide species tend to possess large dipole moments due to charge transfer. Metals have comparably low ionization energies, while CN has a large electron affinity. Thus AlNC has a great deal of Al⁺NC^- character.