Crystalline and porous metal‐organic frameworks (MOFs) are potential candidates for different antibacterial, photocatalytic, and adsorption applications. Moreover, multi‐principal element nanoparticles are effective against multidrug‐resistant bacteria, and combining metals with carbon nanomaterials can enhance activity. In this study, a Tri‐MOF comprised of iron, zinc, and cobalt and 2‐methyl imidazole was grown together with laser‐induced graphene (LIG) powder. Electron microscopy imaging showed the successful preparation and the crystalline nature of the LIG/Tri‐MOF composite. Fourier‐transform infrared and X‐ray photoelectron spectroscopy confirmed a non‐covalent mixture of LIG and Tri‐MOF. Compared with the negligible activity of LIG alone, low doses (0.91‐4.54 mg/mL) of the prepared LIG/Tri‐MOF composite showed excellent antibacterial activity (≥ 95% bacterial removal) and a MIC of 0.6 mg/mL, 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 showed improved antibacterial effects. All materials showed 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 is an essential strategy for minimizing the possible emergence of antibiotic‐resistant strains.This article is protected by copyright. All rights reserved.