Poly(methylsilsesquixoane) network (silicone)-polyimide hybrid materials were successfully prepared by the sol-gel reaction of methyltriethoxysilane (MTES). The ethoxysilyl group in MTES was hydrolyzed and polycondensed in the solution of the polyamic acid, derived from pyromellitic dianhydride and bis(4-aminophenyl)ether, in N,N-dimethyl-acetamide (DMAc). The hybrid films were obtained by casting the reaction mixture, followed by heating up to 300°C. The hybrid materials containing 0-60wt% of silicone afforded flexible films. The films containing less than 7 wt% silicone were yellow and transparent, whereas the films with higher silicone content were yellow and opaque. Silicone particles with a diameter of around 1-10 μm were observed in the fracture surface of the hybrid films by scanning electron microscopy. Although the tensile strength and tensile modulus of the films obtained decreased with increasing silicone content. the value of the elongation at break remained at 60% up to 30% silicone content.