To enhance the mechanical and water barrier properties of soy protein isolate (SPI/)/polyvinyl alcohol (PVA) blends, montmorillonite (MMT), as a layered silicate clay was incorporated and SPI/PVA/MMT composite films were successfully prepared by melt processing in this work. The results showed that the structure of the composites was highly dependent on the MMT content. MMT nanofillers could act as the heterogeneous nucleating agent for PVA, which accelerated the crystallization and increased the size distribution of the crystalline. With the increase of MMT content, the tensile strength and Young's modulus of the composites increased, exhibiting the fine reinforcing effect. Due to the effective restriction of the highly disordered MMT lamellae on the matrix segment, the water sensitivity of the composites decreased and at the same time, the thermal stability improved. The resulting nanocomposite films exhibited wide applications as biodegradable materials, green packaging films, etc. POLYM. COMPOS., 40:3768-3776, 2019. POLYMER COMPOSITES-2019 FIG. 8. The TGA (a) and DTG (b) curves of SPI/PVA/MMT composite films. [Color figure can be viewed at wileyonlinelibrary.com]