have been demonstrated as efficient IFmodified layer for OPV applications, [2] including self-organized molecules, [3] conjugated materials, [2b] ionic compounds (e.g., electrolytes), [4] metal oxides, [1g,5] and nonconjugated organic materials. [6] Typically, the mechanism through which the PCE is improved relies on (i) passivation of interfaces to suppress carrier recombination, [7] (ii) enhanced carrier extraction, [8] (iii) enhancing interfacial dipoles and modifying the work function (built-in dipole) of the electrode to ensure better energy levels alignment, [9] (iv) smoothing the surface of the substrate, [10] and (v) optimizing the blend film morphology. [11] Carbon nanodots (CNDs) are interesting carbon nanomaterials for optoelectronic applications because of their strong luminescence emissions, good water solubility, tunable optical and electronic properties, and photochemical stability. [12] CNDs typically comprise sp 2 -hybridized carbon atoms and present oxygen-containing functional groups (e.g., epoxy, ether, carbonyl, hydroxyl, carboxylic acid) on their surfaces. These oxygen-rich functionalities impart the CNDs with high water dispersibility and make them ready for modification with organic, inorganic, or biological materials. [13] CNDs exhibit interesting photoluminescence (PL) properties because of their sizes, edge shapes, and surface functional groups, and have demonstrated potential applicability in sensing, catalysis, biolabeling, photovoltaic devices, optoelectronic devices, and energy storage. [13d,e,14] CNDs have been employed as active layers, electrolytes, dopants, hole transporting layers, and interfacialmodified layers (IFLs) for dye-sensitized organic and perovskite solar cells. [12] Chen and co-workers first demonstrated the use of amino-based CNDs as efficient zinc oxide (ZnO) or Al-doped ZnO IFLs for OPVs and observed improvements in PCE of up to 10.24%. [13c] Yang et al. used CNDs as a cathode [indium tin oxide (ITO)]-modifying layer that enhanced the interfacial dipole, thereby decreasing the work function (WF) of the electrode and increasing the performance of derived OPV devices from 4.14% to 8.13% when using a poly [4,8bis(5-(2-ethylhexyl)thien-2-yl)benzo [1,2-b:4,5-b′-dithiopheneco-3-fluorothieno[3,4-b]
thiophene-2-carboxylate](PTB7-Th)/ phenyl-C 71 -butyric acid methyl ester (PC 71 BM) blend film as the active layer. [15] These previous studies highlight the potential emerging applications of CNDs as IFLs. CNDs can be prepared