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Inorganic nanomaterials doped with lanthanide ions have been widely used for applications in various fields ranging from biological labeling to solar cells.[1,2]The application of these nanomaterials stems from electronic transitions within rich energy levels of the lanthanide ions, which arise from the tremendous complexity of the 4fn configurations.Subtle changes in the doping concentration, in the form of carefully planned and controlled experiments, can have a dramatic impact on the crystal structure, magnetism, and electronic and optical properties of the resulting materials.Herein, we fabricate a series of lanthanide-doped fluoride nanoparticles with different sizes, and we can tune the upconversion emissions by varying the dopant kinds and doping concentrations, and by designing core-shell nanostructure.