Crosslinked and uncrosslinked ethylene-vinyl acetate copolymer membranes were prepared. The permeation characteristics in the pervaporation process were examined using carbon tetrachloride-acetone mixtures. Modified membranes exhibit carbon tetrachloride permselectivity, but unmodified membranes did not display the permselectivity of crosslinked polymer. Furthermore, membranes modified with dicumyl peroxide (DCP) showed a higher flux and selectivity than those of benzoyl peroxide (BP) modified ones. The effects of feed concentration, molecular size, and polarity of the permeating species on pervaporation were analyzed. The influence of crosslinking density of the membranes on pervaporation was also analyzed. The maximum separation and flux were found to be associated with an optimum amount of crosslinking agent in the membrane. A mixture of chloroform and acetone having a composition near the azeotropic region was also separated by the pervaporation technique.