It is known that polychromatic carbon quantum dots (CQDs) can be obtained by doping and surface modification. The layer-wise synthesis of blue and green emitting CQDs (with typical sizes between 3 and 6 nm) is described here by adding oxalic acid and by introducing polycarboxy groups. By changing the external environment, the emission of CQDs can be adjusted in the blue-green spectral region (469–527 nm) under photoexcitation at 405 nm. The findings presented here provide new directions for the reversible regulatory transformation of polychromatic CQDs. The luminescence also is affected by a variety of conditions such as surface defects, degree of polymerization, polarity of external solutions, and hydrogen bonding which is studied in some detail.