We synthesized carbon quantum dots (CQDs) using a solvothermal method with o-phenylenediamine as the carbon and nitrogen source. The sample was characterized by transmission electron microscopy, X-ray photoelectron spectroscopy, and Fourier transform infrared spectroscopy. When we continued the optical characterization of the CQDs, we were surprised to discover that the colors of the synthesized CQDs changed with the dilution of the original solution. In addition, the photoluminescence (PL) of CQDs under 405 nm continuous wave laser excitation was also investigated. It was found that CQDs with different concentrations exhibited different PL spectra. In order to explain the mechanism of different PL spectra, chemical characterization of the CQDs at different concentrations was performed again, revealing that the color change is independent of particle size and surface functional groups. Systematic optical characterization and theoretical analysis indicate that this color change results from the interparticle distance. Furthermore, we investigated the PL lifetimes of CQDs using time-resolved PL measurements and found that the PL lifetime values change with the concentration of CQDs, which is attributed to nonradiative transitions. Finally, we fabricated warm white-light-emitting diodes with CQDs that are proportionally adjusted in concentrations. The investigation developed a simple and effective method to tune the color of CQDs by adjusting the concentration through dilution of the original solution, which provides a new approach for the preparation and regulation of multicolor CQDs.