Dispersion morphologies of polymer-layered silicate nanocomposites based on either brominated poly(isobutylene-co-para-methylstyrene), BIMSM, or brominated poly(isobutylene-co-isoprene), BIIR, and an organosilicate, dimethylditallow ammonium-exchanged montmorillonite, Cloisite™ 6A, with and without N660 carbon black fillers were examined using SAXS, WAXS, AFM, and TEM. These compounds were prepared using an internal mixer and cured for property measurements. Due to the observed partial orientation of organosilicates and their possible heterogeneous intercalation, degrees of exfoliation and dispersion of organosilicates in BIMSM and BIIR were unable to be characterized and quantified simply by TEM, AFM, or SAXS alone. Instead, using the projected aspect ratio of organosilicates in BIMSM or BIIR, extracted from Gusev-Lusti equation based on measured permeability ratios, was found to provide a relative measure of their dispersion state. Since better dispersion, higher planar orientation, and/or increasing extent of exfoliation lead to higher aspect ratio, this calculated aspect ratio was used as a measure of organosilicate dispersion in BIMSM and BIIR compounds. According to experimentally extracted projected aspect ratios, it was found that BIMSM disperses organosilicates better than BIIR and that carbon black filler does not affect the organosilicate dispersion in BIMSM. Addition of tertiary amines in BIMSM enhances the dispersion of organosilicates, possibly through favorable interactions between organosilicates and quaternary ammonium functionalized BIMSM, resulting in further reduction in permeability.