A series of high‐quality Cu‐doped Zn–In–S nanocrystals (d‐NCs) were prepared by a conventional hot injection process. The full‐visible spectrum emission from 480 to 648 nm can be easily achieved by adjusting the Cu doping concentration in the Zn–In–S system, but not by varying the ratio of In/Zn in the alloyed host material. After wrapping the ZnS shell around the Zn–In–S:Cu d‐NCs core, the resultant Zn–In–S:Cu/ZnS core/shell d‐NCs not only exhibited an enhanced prominent photoluminescent quantum yield (PLQY) up to 65% but also possessed the excellent thermal, photochemical stability, and longer PL lifetime. Furthermore, high color rendition white light was generated from a single color converter Zn–In–S:Cu/ZnS core/shell NCs‐assisted white light‐emitting diodes (LEDs). Under operation of 38 mA forward bias current, the fabricated white LEDs emitted bright natural white light with a luminous efficiency of 62 lm/W, and the correlated color temperature of 5658 K. Simultaneously, the good color stability was accompanied by the CIE color coordinates of (0.3287, 0.3527) under different forward bias currents.