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Bacterial keratitis (BK) is a principal factor contributing to corneal ulcers and ocular complications, and has become a significant killer of global vision health. Traditional antibiotic therapy has unsatisfactory therapeutic effect due to short residence time and low utilization rate of drug, and the long-term abuse of antibiotics can easily incur the prevalence of drug-resistant bacteria. Furthermore, antibiotics are not effective in addressing the excessive inflammatory response caused by infection. Here, we developed a terbium-doped zinc oxide constructed dual-light-responsive nitric oxide (NO)-releasing nanoparticle (ZT@P@B) and modified it on the surface of contact lenses (CL-ZT@P@B) to boost its bioavailability. In vitro and in vivo experimental results verified that ZT@P@B could simultaneously respond to green light (GL) and 808 nm near-infrared (NIR) without obvious damage to the eyes, releasing reactive oxygen species (ROS) and NO, which could effectively kill bacteria (including drug-resistant strains) and reduce inflammatory response. The platform provides a promising strategy for the prevention and treatment of BK.