Endowing metal-organic frameworks (MOFs) with visible-light photocatalytic antiviral and antifungal properties is critical for clean air and healthcare applications, yet challenged by limited biocompatibility and ultraviolet dependency. We herein report a dual strategy of simultaneous amine functionalization and Ti/Ce doping to rationally engineer MOF bandgaps (1.70–2.8 eV) for both white-light antiviral photocatalysis. 20% Ti/Zr-UiO-66-NH2 achieved almost 100% recovery of herpes simplex virus (HSV)-infected cells within 120 min under either 405-nm or white light illumination. Mechanistic studies show a unique •OOH → H2O2 → •OH photocatalytic pathway: photogenerated electrons reduce dissolved O2 to •OOH radicals, which subsequently convert to highly reactive •OH radicals through H2O2, accounting for such excellent antiviral performance. With an energy conversion efficiency of 1.38%, the 20% Ti/Zr-UiO-66-NH2 generated 30% and 169% more •OH radicals than Zr-UiO-66-NH2 and TiO2, respectively. Notably, MOF-based photocatalytic ROS production surpassed traditional non-photocatalytic systems by six orders of magnitude. Our work prospects the molecular-level precision bandgap engineering via ligand/metal doping as an effective pathway to the ration design of highly biocompatible transition metal doped MOF photocatalysts for versatile healthcare applications.