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Highlights Inspired by metalloenzymes with well-defined coordination structures, a series of Cu-X metal–organic frameworks (MOFs) nanozymes with tunable copper active centers were successfully constructed. Experimental and theoretical results strongly supported that precisely tuning the coordination of halogen atoms could directly regulate the enzyme-like activities of Cu-X MOFs by influencing their spatial configuration and electronic structure. The optimal Cu–Cl MOF with excellent enzyme-mimicking activities could effectively relieve ocular chemical burns by possible antioxidant and antiapoptotic mechanisms.