Here, a kind of porous nanoparticles GdAlO₃:Cr³⁺, Sm³⁺ (GAO:Cr,Sm) which own magnetic resonance and long persistent luminescent properties have been synthesized. The spherical morphology and narrow size distribution would allow the GAO:Cr,Sm nanoparticles to be utilised as a drug carrier and the drug release results indicate that the GAO:Cr,Sm drug carriers have an excellent drug sustained properties. Applying the Cr³⁺ and Sm³⁺ coped with gadolinium aluminate as the NIR persistent luminescence center and the energy transfer resonance from Gd³⁺ to Cr³⁺, these nanoparticles exhibit excellent NIR persistent luminescence at 732 nm under the UV irradiation of 254 nm and it can persist for about half an hour. In addition, they possess a longitudinal relaxivity (r1) value of 4.75 mM^-1 s^-1, which means that these nanoparticles could be applied for MR imaging as contrast agents. Carboxymethyl Chitosan was modified on the surface of GAO:Cr,Sm nanoparticles to make them owning excellent biocompatibility and low toxicity and these nanoparticles were successful to realize in vivo imaging. Hence, the well-defined nanoprobes of GAO:Cr,Sm exhibit great potential in biomedicine as trackable drug carriers and in vivo imaging agent due to the dual-model imaging property.