The invention provides a single-particle nano crystal with three-primary-color luminescence and a preparation method thereof. The single-particle nano crystal has a core-shell structure and sequentially comprises an inner core, a first shell, a second shell, a third shell and a fourth shell from inside to outside, wherein the inner core, the second shell and the fourth shell are luminous shells, and the first shell and the third shell are inert shells. The three luminous shells separately contain Yb<3+>/Tm<3+>, Er<3+> or Nd<3+>/Yb<3+>/Er<3+> ions, and the luminescent shells respectively radiate red, green and blue lights under the action of a laser. According to the invention, shell stock solutions with different components are continuously and thermally injected by adopting a one-pot method, and compared with a conventional batch thermal injection method, the one-pot method has the advantages that the time required for synthesizing nano particles with a multilayer core-shell structureis greatly saved. Through constructing a ''core-multi-shell'' structure, concentration quenching and luminescence color crosstalk are inhibited, and high-efficiency pure-color three-primary-color luminescence is realized. The nano crystal has a real-time color adjustment capability in full color gamut, and the adjustment method is simple and convenient.