Carbon dots (CDs) are crystalline, quasi-spherical nanoparticles with sp 2 character and their sizes are in the range of <10 nm. [1][2][3][4][5] Challenging the customary metal based semiconductor quantum dots (SQDs) materials, CDs have emerged as a promising high-tech material for multidisciplinary applications due to their outstanding properties such as chemical inertness, high water solubility, easy surface modification, low or no toxicity, excellent biocompatibility, down-and upconversion-mediated photoluminescence (PL), and high photostability compared to commercial organic dyes, SQDs, and noble metal clusters. [1][2][3][4][5] CDs are versatile PL material; hence, it can be used in a wide range of emerging technologies like bioimaging, [3][4][5][6][7] sensors, [7] lasers, [8] photocatalysis, [9] energy conversion/storage devices, [10] light-emitting diodes, and optoelectronic devices. [11] Luminescent carbon dots (CDs) are emerging as a potential eco-friendly alternative to standard metal-based semiconductor quantum dots. A solvatothermal method to prepare crystalline, nitrogen-rich, surface-passivated, and rare excitation wavelength-independent green-emitting (λ max ≈ 522 nm in solution and 536 nm in solid) CDs from a pyridine diamine precursor in ethanol solvent is reported here. In comparison to a neat thin film of CDs, a film of CD-doped polystyrene microspheres (PS-CDs) displays a remarkable enhancement of the photoluminescence emission intensity driven by optical cavity effect of the composite microspheres. Apart from downconversion onephoton luminescence, upon excitation with 800 nm femtosecond pulse laser, pure CDs and PS-CDs exhibit enhanced upconversion two-photon luminescence in the range of about 410-580 nm.