Bacterial infection is a major problem with diabetic wounds that may result in nonhealing chronic ulcers. Here, we report an approach to antibacterial hydrogel dressings for enhanced treatment of infected skin wounds. A fibrous hydrogel was derived from cellulose nanocrystals that were modified with dopamine and cross-linked with gelatin. The hydrogel was loaded with gentamicin, an antibiotic drug. Enhanced antibacterial hydrogel performance resulted from (i) a highly specific sequestration of Fe ions (much needed by bacteria) from the wound exudate and (ii) a dynamic exchange between gentamicin released from the hydrogel and Fe ions withdrawn from the wound exudate. Such exchange was possible due to the high value of the binding constant of Fe ions to dopamine. The hydrogel did not affect the metabolic activity of skin-related cells and showed enhanced antibacterial performance against common wound pathogens such as and . Furthermore, it promoted healing of infected diabetic wounds due to a synergistic antibacterial effect providing the dynamic exchange between Fe ions and gentamicin. This work provides a strategy for the design of dual-function wound dressings, with both starving and killing bacteria and enhanced wound healing performance.

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