Expeditious evolution of antimicrobial resistance in recent years has been identified as a growing concern by various health organizations around the world. Herein, facile and environmentally benign production of highly antibacterial carbonaceous nanomaterials from Colocasia esculenta and Nelumbo nucifera leaves is reported. After carbonization and oxidative treatment, smaller graphene domains are formed in Colocasia esculenta derivatives, whereas larger sheetlike structures are observed in the case of Nelumbo nucifera. Smaller particle size makes quantum confinement effects more prominent, as is evident in fine‐tuning of the photoluminescence emission after each stage of treatment. The influence of precursor materials on the antibacterial properties of the nanosystems is also demonstrated. When microbiocidal activity was tested against model bacteria Pseudomonas aeruginosa, the nanocomposite derived from Colocasia esculenta leaves showed higher activity than the antibiotic drug clarithromycin (control) with a measured zone of inhibition of 40±0.5 mm. This is one of the highest values reported in comparison with plant‐based carbon–silver nanosystems. Quantitative analysis revealed that the nanocomposite obtained from Colocasia esculenta leaves has antimicrobial efficacy equivalent to those of commercial antibiotic drugs and is able to eradicate bacteria at much lower concentrations than that obtained from Nelumbo nucifera leaves.