The development of antibiotic-independent antimicrobial materials is critical for addressing bacterial resistance to conventional antibiotics. Currently, there is a lack of comprehensive understanding of ionic liquid-modified composites in antimicrobial applications. Here, we innovatively prepared GO-based composites modified with phosphonate ionic liquids via a series of surface functionalizations. The resulting antibacterial composites exhibit significant broad-spectrum activity against both Gram-negative and Gram-positive bacteria, including drug-resistant strains, with stronger efficacy against Gram-negative species. Additionally, the material features excellent long-term reusability and the ability to inhibit/destroy biofilms, which is vital for combating persistent infections. Mechanistic studies reveal its antibacterial effects through multiple pathways: disrupting bacterial membranes, inducing ROS, and inactivating intracellular substances-mechanisms less likely to promote resistance. Overall, these phosphonate ionic liquid-modified polycationic materials demonstrate substantial potential in treating bacterial infections, offering a promising strategy to tackle antibiotic resistance challenges.