Using a 370 nm ultraviolet GaN chip as the excitation light source, white light-emitting diodes (WLED) with a double-layer structure were prepared using blue-green carbon quantum dots/non stoichiometric thiol-ene (CQD/OSTE) and red CdSe/ZnS QD/OSTE composite materials as fluorescence conversion media. When the mass ratio of CQD to OSTE is 1∶6.1, by changing the mass ratio of CdSe/ZnS QD and OSTE composite materials, the color rendering index (CRI) and correlated color temperature (CCT) can be adjusted between 82.3-92.6 and 4231-5478 K, respectively. When the CdSe/ZnS QD: OSTE ratio is 1∶5.4, the CRI of the WLED device can reach 92.6 and the CCT is 5098 K. The prepared WLED devices exhibit good stability under 8 hours of ultraviolet irradiation. This type of WLED device with high color rendering index and stability is expected to be applied in the fields of white light illumination and display.