The present invention relates to methods for the preparation of clay/polymer nanocomposites. The methods include combining an organophilic clay and a polymer to form a nanocomposite, wherein the organophilic clay and the polymer each have a peak recrystallization temperature, and wherein the organophilic clay peak recrystallization temperature sufficiently matches the polymer peak recrystallization temperature such that the nanocomposite formed has less permeability to a gas than the polymer. Such nanocomposites exhibit 2, 5, 10, or even 100 fold or greater reductions in permeability to, e.g., oxygen, carbon dioxide, or both compared to the polymer. The invention also provides a method of preparing a nanocomposite that includes combining an amorphous organophilic clay and an amorphous polymer, each having a glass transition temperature, wherein the organophilic clay glass transition temperature sufficiently matches the polymer glass transition temperature such that the nanocomposite formed has less permeability to a gas than the polymer.