The efficiency and associated environmental impacts of different N-doping strategies of carbon dots (CDs) were evaluated. More specifically, N-doped CDs were prepared from citric acid via two main synthesis routes: Microwave-assisted hydrothermal treatment with addition of N-containing small organic molecules (urea and ethylenediamine (EDA)); and microwave-assisted solvothermal treatment in N-containing organic solvents (n,n-dimethylformamide (DMF), acetonitrile and pyridine). These syntheses produced CDs with similar blue emission. However, XPS analysis revealed that CDs synthesized via both hydrothermal routes presented a better N-doping efficiency (~15 at.%) than all three solvothermal-based strategies (0.6–7 at.%). However, from the former two hydrothermal strategies, only the one involving EDA as a nitrogen-source provided a non-negligible synthesis yield, which indicates that this should be the preferred strategy. This conclusion was supported by a subsequent life cycle assessment (LCA) study, which revealed that this strategy is clearly the most sustainable one from all five studied synthesis routes.