Antibacterial fibers have great potential in numerous applications, including bandages, surgical robes, and surgical sutures, and play a significant role in our everyday lives. Here, zeolitic imidazolate framework‐67 was synthesized using a green method on silk fibers through a layer‐by‐layer process under ultrasonic irradiation (ZIF‐67@silk [U]) and without ultrasonic irradiation (ZIF‐67@silk [B]). Then, iodine was loaded on ZIF‐67@silk samples and were assessed as antibacterial fibers with iodine release. Four samples of ZIF‐67@silk and I2@ZIF‐67@silk were characterized by FT‐IR, PXRD, FE‐SEM, TGA, BET, and UV–Vis spectroscopy. Finally, antibacterial activity of ZIF‐67@silk (B and U) and I2@ZIF‐67@silk (B and U) on Staphylococcus aureus as Gram‐positive bacteria and Escherichia coli as Gram‐negative bacteria was investigated. In addition to ZIF‐67@silk samples, iodine‐loaded samples showed excellent antimicrobial facility.
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