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The authors synthesised porous GdF3 :Er3+, Yb3+ –COOH core–shell structured bi‐functional nanoparticles through a one‐step hydrothermal route during which ethylene diamine tetraacetic acid) was bound to the surface of the nanoparticles. It has high up‐conversion emission intensity for monitoring the drug release process and magnetisation saturation value (10.2 emu/g) for drug targeting under foreign magnetic fields. Moreover, porous GdF3 :Er3+, Yb3+ as drug carriers with a high drug‐loading efficiency. cis‐Dichlorodiammineplatinum(II) (cisplatin, CDDP)‐loaded GdF3 :Er3+, Yb3+ nanoparticles (GdF3 :Er3+, Yb3+ –CDDP) were characterised by the Fourier transform infrared spectra, and CDDP was loaded in the form of electrostatic interaction and hydrogen bonds. Compared with CDDP alone, GdF3 :Er3+, Yb3+ –CDDP nanoparticles increase concentration of CDDP in the target site and enhance its anticancer efficiency. Therefore, the as‐prepared GdF3 :Er3+, Yb3+ –COOH nanoparticles allow simultaneous targeted drug delivery and monitoring as promising anti‐cancer theranostic agents. [ABSTRACT FROM AUTHOR]