The stable Isotope, 34S, was separated at high enrichment by liquid phase thermal diffusion of carbon disulfide in a 12-column, dual cascade system. The first cascade of seven columns was used to separate the mixed molecule, C32S34S, from feed of natural isotopic abundance. Isotopic scrambling of the mixed molecule at high temperature yielded significant amounts of the doubly substituted species, C34S34S. The converted stream was used as feed to a second cascade of five columns from which the C34S34S was extracted as product. Over a period of several months 25.3 g of carbon disulfide was collected at 34S concentrations greater than 91%. Performance of the system was in reasonable agreement with theoretical predictions; however, the measured transport rate of 34S was approximately half of the rate predicted on the basis of recent measurements of the isotopic thermal diffusion factor.