Cyanoformyl chloride and cyanoformyl bromide, XC(O)CN (X = Cl and Br), have been investigated in the gas phase by UV photoelectron and mid-infrared spectroscopies. The ground-state geometries of the neutral molecules have been obtained from quantum-chemical calculations at the B3LYP and CCSD(T) levels using the aug-cc-pVTZ basis set. The individual spectroscopies provide a detailed investigation into the vibrational and electronic character of the molecules and are supported by quantum-chemical calculations. The results are compared to data for structurally and chemically related molecules.