A dual-emission Ce3+-doped LiYF4:Yb3+/Ho3+@LiYF4 upconversion nanoparticles were synthesized. The output color of the nanoparticles can be precisely manipulated by modulating the doping-concentration of Ce3+ ions. Cr3+-responsive rhodamine derivative was assembled on the surface to fabricate the colorimetric probe by LRET process. A sequence of color change were obtained under 980 nm laser excitation, which could easily be visualized by the naked eye. This ratiometric probe is successfully applied to practical detection.