Resistance of pathogens towards commonly used drugs endangers the survival of mankind. Nosocomial infections, increasing treatment duration and costs are already recorded throughout the world. New classes of antimicrobial agents based on natural plant extracts offer valuable solutions due to their naturally evolved synergistic mechanisms in the fight against microorganisms . Aloe Vera Barbadensis Miller (AV) is used since centuries against ailments due to its antimicrobial, anti-inflammatory properties. Iodine is well known and used traditionally as antimicrobial agent, although it has the side effects of skin discoloration and irritation. Another drawback of iodine is the uncontrolled and fast iodine release resulting in short activity. We combined AV gel extract with iodine through a cost-effective and easy one-pot synthesis with polyvinylpyrrolidone (PVP) as encapsulating and stabilizing agent. Smart triiodides with halogen bonding were formed within the PVP matrix by adding iodine (I₂) and sodium iodide (NaI) to the AV-PVP hybrid. Fourier transform infrared spectroscopy (FT-IR) and ultraviolet-visible spectroscopy (UV-Vis) verified the composition of our compounds. The antimicrobial testing by disc diffusion method against 10 reference microbial strains showed excellent to intermediate antimicrobial activity. The triiodide moieties within AV-PVP induced controlled release of iodine and resulted in enhanced microbial inhibition enabling the use as wound care product and skin disinfectants.