The achievement of three-primary-color luminescence in a single material will lead to revolutionary developments of many advanced applications such as dynamic display with ultra-high resolution, and complex anti-counterfeiting. Here we report the realization of steady-state three-primary-color emission in single multilayered NaYF4 upconversion (UC) nanoparticles. In this core-shell structure, a novel design of a tri-sensitizer, i.e., Nd3+, Yb3+ and Er3+ ions, is utilized, which effectively absorbs the excitation photons of 808, 980 and 1550 nm, and then exhibits blue, red and green emissions, respectively. By simply combining the three primary color emissions, tunable full-color luminescence was achieved in this single material. These nanoparticles have demonstrated promising potential applications in dynamic display and multiple anti-counterfeiting.