The formulation of new bionanocomposite (BNC) films using whey protein isolates (WPI, 3.3–11.7 %)-jujube polysaccharide (JPS, 1.59–18.41 %)/starch nanocrystals (SNCs, 0.32–3.68 %) blends was optimized. The ultrasound-assisted acid hydrolysis produced ~63.1 nm SNCs from native starch with −24.3 mV ζ-potential. The extracted JPS purification led to a single symmetrical peak for galactoarabinan-rich fraction (1.35 × 105 Da). The optimal levels of barrier (oxygen (11.85 cm3 m−2 d−1 atm−1) and water vapor (3.22 × 10−10 g m−1 s−1 Pa−1) permeability rate), optical (opacity index (2.7 AU μm−1), total color difference (18.69), and whiteness index (77.40)), and thermal (glass transition temperature (−8.29 °C) and melting point (110.38 °C)) properties were obtained at 5.0 % WPI, 15.0 % JPS, and 3.0 % SNCs. The film-forming solution of optimal BNCs had a significant antibacterial effect against Staphylococcus aureus and Escherichia coli. The improved crystallinity of BNCs at an optimal SNC level was confirmed by the X-ray diffraction (XRD). The field emission-scanning electron (FE-SEM) and atomic force (AFM) microscopy images confirmed a continuous and uniform network for the optimal BNCs without any pores or cracks accompanied by low surface roughness. The FTIR spectroscopy proved covalent interaction and hydrogen bonding among chemical functional groups of WPI and JPS reinforced with SNCs. The optimal BNC could preserve banana fruits with favorable physicochemical and microbial quality during storage.