The action of light on undersaturated and supersaturated vapors of carbon disulfide has been investigated using a batch photochemical reactor and a thermal diffusion cloud chamber, respectively. Photoinduced nucleation was observed in each case. In the batch reactor enough sulfur was produced to nucleate and grow a sulfur aerosol. A model for the photoinduced nucleation of supersaturated carbon disulfide is proposed based upon the photochemical production and subsequent nucleation of sulfur. The model predictions compare well with observed nucleation delay time and nucleation rate data. A variation of the model utilizing diradical polymerization instead of nucleation is used to explain photoinduced nucleation results in the literature involving dilute solutions of carbon disulfide in supersaturated ethanol vapor.