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This study synthesized poly(vinyl alcohol)/carboxymethyl chitosan/cyanidin (PVA/CMCS/CY) hydrogel films. First, PVA and CMCS were used to synthesize hydrogel films by ultraviolet irradiation. Meanwhile, CY was in situ combined into the hydrogel films through the electrostatic attraction between CMCS and CY. Next, the products were analyzed using Fourier-transform infrared spectroscopy, scanning electron microscopy, contact angle test, swelling analysis, and mechanical property test. The results revealed that compared with PVA/CMCS hydrogel films, the PVA/CMCS/CY hydrogel films had an interporous structure and good swelling and mechanical properties. Moreover, the drug release experiments demonstrated that the PVA/CMCS/CY hydrogel films had a CY encapsulation efficiency of 33.5% with a sustained CY release of up to 60 h. Furthermore, the examined antibacterial activities against Staphylococcus aureus and Escherichia coli showed that the porous PVA/CMCS/CY hydrogel films exhibited a certain inhibition. Cell viability experiments demonstrated that the PVA/CMCS/CY films displayed no obvious cytotoxicity to human umbilical vein endothelial cells. [ABSTRACT FROM AUTHOR]