In this study, we fabricated polyvinyl alcohol (PVA)/chitosan (CS) bilayer films by casting and investigated the effects of preparation conditions and CS content (2, 2.5, or 3 wt.%) on the ability of these films to preserve packaged strawberries. The best performance was achieved at a CS loading of 2.5 wt.% (ultrasound time, 25 min); the strain and stress values were 143.15 ± 6.43% and 70.67 ± 0.85 MPa, respectively, oxygen permeability was 0.16 ± 0.08 cm²·m²·day-1·MPa-1, water vapor permeability was 14.93 ± 4.09 g·cm-1·s-1·Pa-1, and the shelf life of fresh strawberries packaged in the PVA/CS 2.5 wt.% bilayer film was determined to be 21 days at 5 ± 2 °C and a relative humidity of 60 ± 5%. Treatment with PVA/CS bilayer films prevented the decrease in the firmness of strawberries during storage (21 days). The evaluated physicochemical parameters (weight loss, decay, firmness, titratable acidity, soluble solid content, ascorbic acid content, and color) indicated that treatment with PVA/CS bilayer films led to better maintenance of the fruit quality. We believe that our study makes a significant contribution to literature because it paves the way to the fabrication of smart packaging materials and facilitates the commercialization of fresh strawberries as an important health food.