The barrier and sorption properties of films based on composites of gelatin and siloxane rubber SKTN-A with additives of montmorillonite (MMT) have been studied. The barrier properties of the films have been evaluated from their permeability to dibromomethane and water by vacuum pervaporation. Using the example of these heteropolar liquids, it has been shown that the permeability of the composites can be regulated by introducing up to 7 wt % MMT into the polymer matrix. The barrier characteristics of the gelatin-MMT composites with respect to dibromomethane have been improved by a factor of 3–4 compared with the original polymer. In the case of a hydrophobic polysiloxane matrix, the effect of organomodified MMT* on the barrier properties is less significant.