The focus of this chapter is the effect of carbon black loading on the resulting fiber structure and tensile properties of thermoset butyl rubber membranes prepared using the electrospinning process. These materials offer potential for use in stretchable, selectively permeable membranes for chemical protective applications. The effect of carbon black loading (0, 25, 50, 75 per hundred parts rubber) on dimensional stability, fiber structure, and mechanical properties was studied. The addition of carbon black filler was found to decrease the fiber diameter and number of beads. Increasing carbon black content decreased the density and tensile modulus. When the tensile properties were corrected for the differences in density, the behavior of the electrospun butyl rubber membranes showed the expected increase with carbon black loading.