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A Unimolecular System Combining Efficient Inhibition of NDM‐1 by Coordination Interactions with High ROS for Synergistically Tackling Drug‐Resistant Bacteria

New Delhi metallo‐β‐lactamase (NDM‐1) that can hydrolyze almost all clinical β‐lactam antibacterial causes “Super” bacterial infection, which seriously threatens human health worldwide. Therefore, it is urgent to establish powerful methods for inhibiting NDM‐1 activity and efficient anti‐resistant bacteria. Herein, a new strategy for the depression of NDM‐1 activity and synergistic therapy to overcome drug‐resistant bacteria based on conjugated oligomer (OPV)‐modified porphyrin derivatives OPV‐C6‐TPP probe is developed. The unimolecular probe not only can coordinate Zn2+ in NDM‐1 to suppress the activity of NDM‐1 but also produce the high 1O2 under light irradiation, providing dual functions of activating antibiotics and photodynamic therapy. The chelation inhibition mechanism of OPV‐C6‐TPP on NDM‐1 is investigated and further confirmed by molecular docking and molecular dynamics simulation studies. In the presence of probe, the minimum inhibitory concentration of antibiotic model cefazolin is reduced ≈50 times, significantly reversing resistance and resensitizing NDM‐1‐overexpressing Escherichia coli (E. coli‐NDM‐1) to antibiotics. Furthermore, the combined system greatly accelerates wound healing in E. coli‐NDM‐1 infected mice due to photodynamic and antibiotic synergistic effects. This study paves the way for the efficient treatment of drug‐resistant bacteria.