CS was discovered by Béla Lengyel, who assigned it an unsymmetrical structure. Later, infrared and Raman spectroscopy showed that the structure is symmetrical with a D point group symmetry, i.e. S=C=C=C=S. This compound is analogous to carbon suboxide whose structure is O=C=C=C=O.
Lengyel first synthesized this compound by passing carbon disulfide (CS) vapor through an electric arc with carbon electrodes. This treatment produced a black solution that after filtration and evaporation gave a cherry-red liquid. He determined the molecular mass by cryoscopy. Later preparations of CS include thermolysis of a stream of CS in a quartz tube heated to 900 to 1100 °C as well as flash vacuum pyrolysis (FVP) of 1,2-dithiole-3-thiones.