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With the objective of creating an electro‐responsive and antimicrobial device suitable as delivery system for Rose Bengal (RB) to the skin, a hybrid hydrogel combining Chitosan (CS) and Graphene Oxide (GO) are designed, serving as functional polymer support and active filling element, respectively. The hybrid system, synthesized using tripolyphosphate as a crosslinker via ionic gelation, shows a uniform and homogeneous surface, as verified by SEM investigations, high biocompatibility when tested on human fibroblast lung cells MRC‐5 cells, and biodegradability in phosphate buffered medium at physiological pH. Drug loading and release experiments, extensively analyzed using suitable mathematical modeling, shows the enhancement of the binding efficiency conferred by GO (534 and 979 mg g−1 for blank and hybrid hydrogels, respectively) and an electro‐responsive behavior (maximum BR release of 36 and 23% at 0 and 12 V, respectively). Additionally, hybrid hydrogel is found to prevent the adhesion of methicillin‐resistant Staphylococcus aureus and to kill the bacterial cells by taking advantage of the sustained release of the antimicrobial RB. [ABSTRACT FROM AUTHOR]