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Abstract: Pea starch nanocrystals (PSN) dispersion containing nanocrystals in a range of 30–80nm was prepared from native pea starch (NPS) granules by acid hydrolysis. Two series of films were prepared by blending poly(vinyl alcohol) (PVA) with NPS and PSN, respectively. The effects of NPS and PSN on the structure and properties of the resulting films were comparatively investigated by FTIR, XRD, SEM, and testing of light transmittance, tensile, and moisture uptake. The light transmittance (Tr), tensile strength (σ b), and elongation at break (ε b) of the PVA/NPS films were lower than that of PVA film and decreased with an increase in NPS content. However, the PVA/PSN nanocomposite films containing 5 and 10wt% of PSN content exhibited improved physical properties over the PVA film. The PVA/PSN films showed higher Tr, σ b, and ε b, and lower moisture uptake (Mu) than the corresponding PVA/NPS films with the same component ration. For example, the values of Tr, σ b, ε b, and Mu of the PVA/PSN film containing 10wt% of PSN content were 91%, 40MPa, 734% and 71%, respectively; while those of the corresponding PVA/NPS film were 69%, 35MPa, 579% and 73%, respectively. The results revealed that PSN, comparing with NPS, had much smaller sizes and dispersed more homogeneously in PVA matrix, resulting in stronger interactions with PVA. New applications of native pea starch and its nanocrystals as low-cost fillers were explored in this work, and PSN exhibited greater potential than NPS to improve the properties of PVA-based composites. [Copyright &y& Elsevier]