We have prepared nanocomposites of intercalated and exfoliated organosilicates in butadiene rubber (BR) by using a two-stage melt blending process. We used X-ray diffraction and transmission electron microscopy to examine, respectively, the intergallery spacing of the organosilicates and their dispersion in the BR. Marked enhancements in the mechanical and thermal properties of BR occurred when it incorporated <10 parts of organosilicates and the loading ratio of the organosilicate to dicarboxylic acid-terminated butadiene oligomer was approximately three. In particular, the addition of 10 parts of organosilicate and 3 parts of compatibilizer in the BR led to a more than four-fold increase in the tensile strength, a 150% increase in modulus at 100% elongation (M100), and 232 and 410% enhancements in the tear strength and elongation at break, respectively, relative to those of neat BR. The degradation temperature for the BR nanocomposite containing only a 10-part loading of organosilicate was 51 °C higher than that of neat BR; these increases reduced, however, to 9-13°C upon the addition of the CTB compatibilizer. In addition, the relative water vapor permeabilities of the BR nanocomposites containing 10 parts of organosilicate-both in the presence and absence of the compatibilizer-reduced to 20% of that of the neat BR.