A series of protein-based biocomposites was prepared from glycerol-plasticized zein (ZE) and pea protein isolate (PPI) using a hot press and moulding process. The effects of PPI content (W-PPI) on the structure and properties of ZE/PPI films were investigated. With an increase in W-PPI from 0 to 100%, the elongation at break of the films increased from 2.4 to 62.6%, and the water contact angle decreased from 31.8 degrees to 5.8 degrees. Cell toxicity and cytocompatibility of ZE/PPI films were evaluated in vitro. The cell viability of L929 cells cultured in extracts from ZE/PPI films containing 10-30% PPI was higher than that from other films and the control group. The L929 cells expanded very well on the surfaces of films containing 10-30% PPI. Incorporation of 10-30% PPI into ZE improved flexibility, surface hydrophilicity, cytocompatibility and its potential as biomaterials in zein-based composites.