Lanthanide doped bifunctional materials are potentially important for developing multifunctional devices. Here, NaLuF4:Yb3+/Tm3+/Gd3+/Sm3+ optical-magnetic bifunctional microcrystals were successfully synthesized by hydrothermal method, which could emit ~480 nm blue light from the1G4→3H6 electronic transition and ~800 nm infrared light from the3H4→3H6electronic transition of Tm3+ ion, under the excitation of 980 nm infrared light. By doping Sm3+ ion into NaLuF4:Yb3+/Tm3+/Gd3+, the infrared emission peak centered at 800 nm would shift obviously to longer wavelength. This indicated that Sm3+ ion could efficiently tune the energy level gaps of Tm3+ ions in NaLuF4 host which was demonstrated based on the crystal field theory. In addition, these NaLuF4:Yb3+/Tm3+/Gd3+/Sm3+ microcrystals presented unique ferromagnetic property instead of usually reported paramagnetic prop-erty. Importantly, the ferromagnetic property decreased with increasing the concentration of Gd3+ ion. This was in good agreement with Swift’s theoretical investigation that the coexistence of light rare earth (Gd3+) and heavy rare earth (Yb3+/Tm3+) would lead to the anti-ferromagnetic coupling in the sub-lattices.
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