As the foremost category of carbon materials, carbon dots (CDs) have been extensively applied in many domains because of their special fluorescence features and outstanding biocompatibility. However, in early studies of fluorescent CDs, as the fluorescence wavelength of most CDs was restricted to the blue or green region and was excitation dependent, the application of CDs was limited. In this study, three representative CDs, fluorescing yellow, green, and blue, were synthesized under alkaline, neutral, and acidic circumstances, respectively, while using a hydrothermal method in which catechol and phthalaldehyde acted as carbon sources and methanol functioned as the reaction solvent. The carbon nuclei of the three fluorescent CDs all had comparable graphite structures. The diversity of photoluminescence (PL) emission from these three CDs was attributed mainly to the different sizes of the sp² conjugated structures among them. Mixing synthesized CDs with epoxy resin, three colors (yellow, green, and blue) of LED using CIE coordinates (0.40, 0.44), (0.33, 0.46), and (0.21, 0.22), respectively, were successfully prepared.