In this paper, the mechanical properties of PI/SiO2 nanocomposite hybrid films with different silica doping levels are experimentally studied at low temperature. Experimental results show that the coefficient of thermal expansion (CTE) of the PI/SiO2 nanocomposite hybrid films gradually reduces when the ambiance temperature is decreased. At the liquid nitrogen temperature (77K), the CTE value is about five times less than that at room temperature (287K). The measured CTEs of hybrid films greatly decrease when doped with inorganic silica, especially when the silica doping level is more than 1wt.%. However, too high silica contents (more than 10wt.%) can cause problem to disperse effectively and the specimens become quite opaque. Experimental results also show that the effects of the pre-applied stress levels can be neglected on the CTE testing. When the ambient temperature changes from 287 to 77K, the measured average values of the films' ultimate tensile strength (UTS) and Young's modulus increase about 60 and 90%, respectively, while the breaking elongation decreases about 42%.