This paper presents work on the green synthesis of the graphene quantum dots (GQDs) and carbon dots (CDs) from leaves of Erythrina caffra (E. caffra) using a simple technique to facilitate the carbonization process, from methanol and water extracts of E. caffra leaf, and their evaluation as potential antiviral agents against SARS-CoV-2. Phytochemical profiling of E. caffra leaf extracts exhibited the presence of phenols, alkaloids, steroids/terpenoids, tannins, and flavonoids. FTIR analysis confirmed the incorporation of oxygenated functional groups inherited from the phytochemicals. UV-Vis indicated the presence of secondary metabolites in both extracts and CDs. X-ray diffraction spectra confirmed the amorphous and crystalline nature of synthesized CDs (2.51 nm) from water extracts and GQDs (0.08 nm) from methanol extracts. The CDs and GQDs exhibited respective sizes of 5.5 and 4.0 nm, with a dot-like morphology, and respective zeta potential of +200.0 and −12.6 mV. The results revealed that all extracts and carbon dot formulations exhibited high cell viability (>90%), indicating excellent biocompatibility and minimal cytotoxicity at the tested concentration of 100 mg/mL per sample. The SARS-CoV-2 experiments demonstrated that extracts (MeOH, H₂O) and nanomaterials (CDs-H₂O, GQDs-MeOH) exhibited a virus suppression efficacy of 87.86 ± 4.75%, 87.95 ± 0.77%, 87.95 ± 3.08%, and 94.84 ± 0.94%, respectively. All examined samples demonstrated viral inhibition over 88%. Both extracts and their respective nanomaterials showed that a minimum of 5 μg was required to achieve 50% antioxidant species per sample. The study highlights E. caffra as a sustainable precursor for eco-friendly carbon dot synthesis as potential antiviral and antioxidant candidates.