In this study, we report a metallogel developed based on metal-phenolic coordination of natural low-cost polyphenolic molecule and metal ions. Gelation occurs by mixing tannic acid (TA) and group (IV) titanium ions (Ti IV ) to form TA-Ti IV gel. The TA-Ti IV gel exhibits good capability to incorporate diverse metal ions by in situ co-gelation. Herein, five antimicrobial metal ions, i.e. ferric (Fe III ), copper (Cu II ), zinc (Zn II ), cobalt (Co II ) and nickel (Ni II ) ions, were employed to include in TA-Ti IV gels for developing intelligent dressings for infected wounds. The chemical and coordinative structures of TA-Ti IV metallogels were characterized by UV-Vis and Fourier-transform infrared (FT-IR) spectroscopies. Cytotoxicity of antimicrobial metallogels was explored by MTT assay with NIH 3T3 fibroblasts. The release of metal ions was evaluated by inductively coupled plasma mass spectrometry (ICP-MS), indicating the different releasing profiles upon the coordinative interactions of metal ions with TA. The formation and disassembly of metallogels are sensitive to the presence of acid and an oxidizer, H 2 O 2 , which are substances spontaneously generated in infected wounds due to the metabolic activity of bacteria and the intrinsic immune response. The Cu II releasing rates of TA-Ti IV -Cu II metallogels at different pH values of 5.5, 7.4 and 8.5 have been studied. In addition, addition of H 2 O 2 trigger fast release of Cu II as a result of oxidation of galloyl groups in TA. Consequently, the antimicrobial potency of TA-Ti IV -Cu II metallogels can be simultaneously activated while the wounds are infected and healing. The antimicrobial property of metallogels against Gram-negative Escherichia coli , and Gram-positive Methicillin-Resistant Staphylococcus aureus (USA300) and Staphylococcus epidermidis has been investigated by agar diffusion test. In an animal model, the TA-Ti IV -Cu II metallogels were applied as dressings for infected wounds, indicating faster recovery in the wound area and extremely lower amount of bacteria around the wounds, compared to TA-Ti IV gels and gauze. Accordingly, the intelligent nature derived metallogels is a promising and potential materials for medical applications.