Abstract Cyanogen isocyanate (NC–NCO) has been prepared and studied using a combined experimental and theoretical approach. A crystalline film of the interpseudohalogen species was stabilized by vapor deposition on a cold substrate (T=–100 C). From IR spectroscopy on the “free” molecule, trapped in a matrix of solid argon, the connectivity and geometry of this unstable interpseudohalogen was deduced and ...