The energy-upconversion of lanthanide-doped nanoparticles with a core-shell structure can be utilized to enhance and tune optical properties and can generate multifunctionality in a single system. Herein, the core-shell nanoparticles NaYF4:Yb,Ho,Tm@NaGdF4 were prepared by thermally decomposing lanthanide acetylacetonate precursors. Through modifying the molar ratio of the core and shell, nanodumbbell-shaped particles with different sizes and morphologies were precisely synthesized. The formation mechanism and the heterogeneous epitaxial growth process of the nanodumbbell-shaped particles were studied. After coating the shell layer, upconversion luminescence intensities, spectral purity and fluorescence lifetimes were improved. Furthermore, the magnetic performance of the core-shell nanoparticles was characterized. The optical-magnetic bifunctional upconversion core-shell particles with programmable shape and multiple properties provide an ideal platform for the preparation of nanodumbbell-shaped particles and the promotion of upconversion materials for biomedical research.