The enhancement in the emission of visible light in the synthesized coaxial ZnO@ZnS core-shell nanorods (CSNR) has led to the development of a nearly white light-emitting photoluminescent material as confirmed by the calculation of Commission Internationale de l'Eclairage chromaticity coordinates. However, we have fabricated a nearly white light-emitting diode (WLED) by combining a commercial UV LED chip with our CSNR material, and it emits warm white light. The observed increase in the relative intensity of deep level (IDLE) over UV (IUV) photoluminescence emission is attributed to the addition of new defect states during the formation of the shell with a larger thickness as becomes evident from X-ray photoelectron spectroscopy (XPS) study. Thanks to the presence of such defect states, whose effective exploitation enabled us to obtain ~93% photodegradation of a test dye, namely, methylene blue, in the presence of core-shell ZnO@ZnS heterostructure within only 25min of irradiation of UV-Visible light. Thus, apart from demonstrating the fabrication of a near WLED, we have successfully demonstrated the enhanced photocatalytic performance by tweaking the surface defects of ZnO nanorods via the formation of coaxial ZnO@ZnS core-shell nanorods with various shell thicknesses. [ABSTRACT FROM AUTHOR]