In chronic wounds, the regeneration process is compromised, which brings complexity to the therapeutic approaches that need to be adopted, while representing an enormous loss in the patients’ quality of life with consequent economical costs. Chronic wounds are highly prone to infection, which can ultimately lead to septicemia and morbidity. Classic therapies are increasing antibiotic resistance, which is becoming a critical problem beyond complex wounds. Therefore, it is essential to study new antimicrobial polymeric systems and compounds that can be effective alternatives to reduce infection, even at lower concentrations. The biological potential of polyphenols allows them to be an efficient alternative to commercial antibiotics, responding to the need to find new options for chronic wound care. Nonetheless, phenolic compounds may have some drawbacks when targeting wound applications, such as low stability and consequent decreased biological performance at the wound site. To overcome these limitations, polymeric-based systems have been developed as carriers of polyphenols for wound healing, improving its stability, controlling the release kinetics, and therefore increasing the performance and effectiveness. This review aims to highlight possible smart and bio-based wound dressings, providing an overview of the biological potential of polyphenolic agents as natural antimicrobial agents and strategies to stabilize and deliver them in the treatment of complex wounds. Polymer-based particulate systems are highlighted here due to their impact as carriers to increase polyphenols bioavailability at the wound site in different types of formulations.