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Herein, a thermally responsive donor of cell\u2010messenger nitric oxide (NO) is combined with extracts of food\u2010grade <jats:italic>Lactobacillus casei<\/jats:italic> to form biomimetic phage\u2010like microparticles with a tailspike structure. These particles can invade bacterial membranes and release NO to disrupt nitrogen and respiratory metabolisms, which initiates the programmed death of multidrug\u2010resistant <jats:italic>Staphylococcus aureus<\/jats:italic> (MRSA) for inducing lysis, like the bacterial virus. Experiments suggest that these microparticles can also weaken bacterial toxicity and provide favorable conditions for cell proliferation because of the continuously released NO. By encapsulating these microparticles into graphene\u2010oxide\u2010doped polymers, a dual\u2010mode antibacterial hydrogel (DMAH) can be constructed. 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