Carbon dots (CDs) are synthesized by the solvothermal method with four kinds of solvents including water, dimethylformamide (DMF), ethanol, and acetic acid (AA). The aqueous solutions of the above CDs emit multiple colors of blue (470 nm), green (500 nm), yellow (539 nm), and orange (595 nm). The structures, sizes, and chemical composition of the CDs are characterized by transmission electron microscopy (TEM), dynamic light scattering (DLS), X-ray diffraction (XRD), Fourier transform infrared (FTIR), and X-ray photoelectron spectroscopy (XPS). The optical properties of multicolored CDs are analyzed by UV-vis absorption and photoluminescence (PL) spectra. It has been revealed that DMF is the key solvent to synthesized CDs for the red shift of fluorescence emission, which could be enhanced by adding an AA solvent. The structures of functional groups such as the contents of graphitic N in carbon cores and oxygen-containing functional groups on the surface of CDs are affected by these four solvents. According to the oxidation and selective reduction of NaBH, the implication for multicolor imaging has been discussed based on the COOH, C-O-C, and C=O functional groups.