A growing number of device-related nosocomial infections, elevated hospitalization costs, and patient morbidity necessitate the development of novel antibacterial strategies for clinical devices. We have previously demonstrated a simple, aqueous polydopamine dip-coating method to functionalize surfaces for a wide variety of uses. Here, we extend this strategy with the goal of imparting antifouling and antimicrobial properties to substrates, exploiting the ability of polydopamine to immobilize polymers and induce metal nanoparticle formation. Polydopamine was deposited as a thin adherent film of 4 nm thickness from alkaline aqueous solution onto polycarbonate substrates, followed by grafting of antifouling polymer polyethylene glycol and in situ deposition of silver nanoparticles onto the polydopamine coated polycarbonate substrates. Elemental and morphological surface analyses confirmed successful grafting of polyethylene glycol brushes onto polydopamine-coated substrates, as well as spontaneous silver nanoparticle formation for polydopamine-coated substrates incubated in silver-nitrate solutions. Sustained silver release was observed over at least 7 days from silver-coated substrates, and the release kinetics could be modulated via additional polydopamine overlayers. In vitro functional assays employing gram negative and positive strains demonstrated dual fouling resistance and antibacterial properties of the coatings due to the fouling resistance of grafted polyethylene glycol and antibacterial effect of silver, respectively. Polycarbonate substrates coated only with silver using a method similar to existing commercial coatings provided an antibacterial effect but failed to inhibit bacterial attachment. Taking into account the previously demonstrated substrate versatility of polydopamine coatings, our findings suggest that this strategy could be implemented on a variety of substrate materials to simultaneously improve antifouling and antimicrobial performance.