Optical-magnetic (OM) bifunctional materials are of great interest for developing advanced multifunctional devices. [1][2][3][4] Conventional OM bifunctional materials are composites that are produced by coupling optical materials with magnetic ones. It is very difficult to realize an interaction between the optical and magnetic properties (e.g., tuning the optical properties using a magnetic field) in these conventional OM materials because of the separation of the optical and magnetic phases. On the other hand, producing materials with OM interactions would be valuable for developing advanced OM devices for high-accuracy communications, aircraft guidance, and magnetic field detection. [4][5][6][7] OM interactions depend mainly on the outermost electrons and thus, occur at the atomic scale. To achieve an OM interaction, a single-phase material should simultaneously have optical and magnetic properties to ensure the OM interaction occurs between atoms in the same crystal lattice, not at the interface between two separated phases with a high density of defects.Recent reports show that OM interactions can be simultaneously observed in single-crystal or single-phase materials by lanthanide (Ln) doping, for example, NaGd-F 4 :Yb 3+ ,Er 3+ [8, 9] and Gd 2 O 3 :Yb 3+ ,Er 3+ . [6,10] The host materials containing Gd 3+ ions have paramagnetic properties while the doped Er 3+ ions form luminescent centers. [6,[8][9][10] The luminescence of Er 3+ ions depends on their coordinated magnetic ion, Gd 3+ . Therefore, if the impact of the coordinating magnetic ions on their luminescent centers is strong enough, they should change the luminescence of these lanthanide-doped materials depending on the magnetic field.In comparison to Gd 2 O 3 , NaGdF 4 has a lower matrix phonon energy so that it generates a higher luminescent efficiency. [11] Moreover, for NaLnF 4 structures, heavy doping of other lanthanide ions does not usually generate precipitating phases. Considering its advantages, we chose NaGdF 4 as the host material to dope with the classic upconversion ionic pair, Yb 3+ /Er 3+ , which can convert low-energy infrared (IR) photons to higher-energy visible light. To adjust the OM properties, an Nd 3+ ion was introduced into the NaGd-