The interfacial properties of a homopolymer (polybutadiene (PB)) and a terpolymer (brominated poly(isobutylene-co-p-methylstyrene) (BIMS)) are reported. Neutron reflectivity was used to study the interfacial structure. The results were complemented by scanning transmission X-ray microscopy and atomic force microscopy, which were used to probe the morphology of these binary blends. Our results show that the interfacial behavior of these elastomeric blends is a direct function of the BIMS chemical composition. The interfacial width decreased with increasing bromide functionality. At levels below 8 mol%, the para-methylstyrene concentration had a less pronounced effect on the compatibility and interfacial characteristics. We also studied the effect of styrene butadiene random copolymers on the miscibility of the PB/BIMS blends. The results showed that styrene-butadiene rubber (SBR) was not fully miscible with BIMS and PB on an individual basis, but addition of relatively small amount of SBR enhances the compatibilization of the PB/BIMS interface. Self-consistent field (SCF) modeling was used to determine the optimum copolymer composition. The calculations are consistent with the experimental results.