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The exploration of strategy to synthesize nanofibril film for functional applications is of great scientific and technological interest. This paper demonstrates that nanofibril film, made of biodegradable konjac glucomannan (KGM) and polyethylene oxide (PEO), performs better physical and chemical properties than solvent casting film. We fabricate a nanofibril film by electrospinning method. To collect consistent and uniform nanofibers, we explore the effect of the proportion of KGM and PEO. At proportion of KGM: PEO = 1:10, the as-prepared nanofibers are consistent in size with an average width of 200 nm. We further characterize the nanofibril film by Fourier transform infrared spectrum (FT-IR) and X-ray diffraction (XRD). The results show physical crosslinked networks between KGM and PEO chains, and modifications of the crystallization of the polymers. In addition, we disperse grape seed extract (GSE) into the electrospinning solutions to prepare bioactive nanofibril film. The as produced nanofibril film demonstrates good water vapor barrier and antioxidation function.