In this manuscript, we describe the fabrication of photoactive biocidal or sporicidal films from urea-derived graphitic carbon nitride (u-g-C3N4). Co-deposited films of u-g-C3N4 and Escherichia coli O157:H7 (IC50 = 14.1 ± 0.2 mJ) or Staphylococcus aureus (methicillin resistant IC50 = 33.5 ± 0.2 mJ, methicillin sensitive IC50 = 42.7 ± 0.5 mJ) demonstrated significantly enhanced bactericidal behavior upon administration of visible radiation (400 nm ≤ λ ≤ 426 nm). In all cases, complete eradication of the microbial sample was realized upon administration of 100 mJ of visible radiation, while no antimicrobial activity was observed for non-irradiated samples. In contrast, Bacillus anthracis endospores were more resistant to u-g-C3N4 mediated killing with only a ca. 25% reduction in spore viability when treated with a 200 mJ dose of visible radiation. Characterization of u-g-C3N4 reveals that the improved activity results from enhancements of both the surface area and reduction potential of the material’s conduction band edge, coupled with fast injection of charge carriers into localized states and a decline in radiative recombination events. The results of this study demonstrate that g-C3N4-based materials offer a viable scaffold for the development of new, visible light driven technologies for controlling potentially pathogenic microorganisms.