Organosoluble montmorillonite/polyimide hybrids were prepared using a monomer solution intercalation polymerization method. Montmorillonite was organo-treated with p-aminobenzoic acid and the organosoluble polyimide was based on pyromellitic dianhydride and 4,4＇-diamino-3,3＇-dimethyldiphenylmethane. The particle size of montmorillonite in the hybrid containing 1 wt % of montmorillonite is about 400 nm. The strength and the toughness of montmorillonite/polyimide hybrids are improved simultaneously when the montmorillonite content is below 5 wt %. The thermal stabilities of montmorillonite/polyimide hybrids are obviously improved and their thermal expansion coefficients are reduced. When the montmorillonite content is below 5 wt %, the montmorillonite/polyimide hybrids are soluble in strong aprotonic polar organic solvents.