The adjustment of the emitting wavelength of carbon dots (CDs) is usually realized by changing the raw materials, reaction temperature, or time. This paper reported the effective synthesis of multicolor photoluminescent CDs only by changing the solvent in a one-step solvothermal method, with 1,2,4,5-tetraaminobenzene as both the novel carbon source and nitrogen source. The emission wavelengths of the as-prepared CDs ranged from 527 to 605 nm, with quantum yields (QYs) reaching 10.0% to 47.6%, and it was successfully employed as fluorescence ink. The prepared red-emitting CDs (R-CDs, λem = 605 nm) and yellow-emitting CDs (Y-CDs, λem = 543 nm) were compared through multiple characterization methods, and their luminescence mechanism was studied. It was discovered that the large particle size, the existence of graphite Ns, and oxygen-containing functional groups are beneficial to the formation of long wavelength-emitting CDs. Y-CDs responded to crystal violet, and its fluorescence could be quenched. This phenomenon was thus employed to develop a detection method for crystal violet with a linear range from 0.1 to 11 µM and a detection limit of 20 nM.