Polyimide (PI) films equipped on the surface of spacecraft are susceptible to ultraviolet damage. Herein, the performance of two kinds of polyimide films i.e. 3,3 ',4,4 '-biphenyl dianhydride-p-phenylenediamine (BPDA-PDA) and pyromellitic dianhydride-4,4 '-oxydianiline (PMDA-ODA) under vacuum ultraviolet (VUV, 172 nm) irradiation was studied. The failure behavior of the PI films was studied by tensile tests, thermogravimetry (TGA), thermomechanical analysis (TMA), electric breakdown, UV-visible transmittance and scanning electron microscopy (SEM). Fourier transform infrared spectroscopy (FTIR) and X-ray photoelectron spectroscopy (XPS) were used to analyze the molecular structure. The results indicated that the tensile strength of BPDA-PDA PI and PMDA-ODA PI films decreased by 10.4 and 7.4% under VUV irradiation, respectively; the breakdown strength and UV-transmittance also deteriorated. Besides, the surface morphology of the PI films showed a large number of microcracks after VUV irradiation, which we ascribe to the breakage of imide rings (C-N-C) and ether bonds (C-O-C) of the PI films. However, the thermal stability (residual weight) of both PI films remained constant compared to the initial level; this can be explained by the combined effect of bond breaking and cross-linking of the polyimide films.