Multifunctional Pr3+-doped GdPO4 nanocrystals possessing UV, visible emissions and magnetic properties were synthesized via co-precipitation and following annealing. It was revealed that as-prepared GdPO4 nanorods were transformed to nanoparticles after heat treatment at 900 °C for 2 hours. Ultimately, GdPO4:Pr3+ nanoparticles have strong UV emission under the excitation of 275 nm and visible emission under the excitation of 445 nm, which offers the optical modalities in both UV and visible range. Moreover, Gd3+-containing nanoparticles are efficient T
-weighted (negative) magnetic resonance (MR) contrast agents due to the presence of Gd3+ ions, which can be potentially applied as multimodal, photoluminescence-magnetic resonance imaging contrast agent.