High-quality InP/ZnS core–shell nanocrystals with luminescence tunable over the entire visible spectrum have been achieved by a facile one-pot solvothermal method. These nanocrystals exhibit high quantum yields (above 60%), wide emission spectrum tunability and excellent photostability. The FWHM can be as narrow as 38 nm, which is close to that of CdSe nanocrystals. Also, making use of these nanocrystals, we further demonstrated a cadmium-free white QD-LED with a high color rendering index of 91. The high-performance of the resulting InP/ZnS NCs coupled with their low intrinsic toxicity may further promote industrial applications of these NC emitters.