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Crystalline and porous metal–organic frameworks (MOFs) are potential candidates for different antibacterial, photocatalytic, and adsorption applications. Moreover, multiprincipal element nanoparticles are effective against multidrug‐resistant bacteria, and combining metals with carbon nanomaterials can enhance activity. Herein, a Tri‐MOF comprised of iron, zinc, cobalt and 2‐methyl imidazole is grown together with laser‐induced graphene (LIG) powder. Electron microscopy imaging shows the successful preparation and the crystalline nature of the LIG/Tri‐MOF composite. Fourier‐transform infrared and X‐Ray photoelectron spectroscopy confirm a noncovalent mixture of LIG and Tri‐MOF. Compared with the negligible activity of LIG alone, low doses (0.91–4.54 mg mL−1) of the prepared LIG/Tri‐MOF composite show excellent antibacterial activity (≥95% bacterial removal) and a MIC of 0.6 mg mL−1 for Gram‐negative bacteria, via the gradual leaching of metal ions and organic linker from the material enhanced by bacterial aggregation near the LIG/Tri‐MOF. Compared to a mixture of separately synthesized Tri‐MOF and LIG, the LIG/Tri‐MOF composite shows improved antibacterial effects. All materials show cytotoxicity for L929 mouse cell lines, the solids showing a disrupting effect on cells grown in vitro. Performance‐enhancing combinations of various materials leading to synergistic or additive antimicrobial effects are essential strategies for minimizing the possible emergence of antibiotic‐resistant strains. [ABSTRACT FROM AUTHOR]