Dispersed polymer/clay nanocomposites are of great interest because they can offer significant property enhancements. Achieving a high level of clay dispersion has been a key challenge. In this paper, we explore a novel supercritical carbon dioxide (scCO2) processing method that utilizes scCO2 to disperse nano-clays. The structure and properties of the clays and the resultant nanocomposites are characterized using a combination of wide-angle X-ray diffraction (WAXD), Scanning Electron Microscopy (SEM), Transmission Electron Microscopy (TEM), and rheology. Our results indicate that nano-clays can be delaminated by the scCO2 process and the extent of dispersion is dependent on the CO2-philicity of the nano-clay. Significant dispersion was achieved with Cloisite 93A, whereas relatively little dispersion was achieved for Cloisite Na+. It appears that the presence of an acidic hydrogen on the ammonium salt (as in the case of 93A) or an increased positive charge on the N of the ammonium salt (I-30P) increases the CO2-philicity of the nano-clay and therefore increases dispersion. In addition, results demonstrate that natural clay (Cloisite Na+) can be dispersed by combining CO2-philic PDMS with the clay prior to processing. We have prepared PDMS/clay, PS/clay and PVME/clay nanocomposites via scCO2 processing, using natural or organically modified montmorillonite clays. The nanoclays and nanocomposites are characterized using WAXD, Rheology and DSC. Our results suggest that we can disperse nanoclays to a significant extent, depending on the ‘CO2 philicity' of the clay. In fact, a CO2-philic polymer may be able to enhance clay dispersion. For PS/clay nanocomposites, the high degree of dispersion achieved through sc-CO2 appears to result in an order of magnitude increase in the rheological properties of PS, associated with an increase in the Tg of around 13˚C, at 10% clay loading. These moduli improvements are significant better than those obtained with conventional, chemically-modified intercalated clay nanocomposites. The degree of enhancement in the properties appears to be strongly dependant on the polymer-clay interactions, and how it is promoted by the supercritical fluid. In the case of PDMS nanocomposites, where the clay-polymer interactions were weak, the modulus increase at low frequencies (for sc-CO¬2 processed system) was only a factor of 2. Our results indicate that scCO2 can not only disperse nanoclays in polymers, it can also significantly enhance clay-polymer interactions.