Rare earth ion-doped fluoride upconversion nanoparticles (UCNPs), emerging as a novel class of probes and drug carriers, exhibit superior promise for bio-applications in diagnostics and treatment on account of their strong luminescence, fine biocompatibility, and high drug loading. However, the fine control and manipulation of particle size and the distribution of rare earth ion-doped oxides has remained an insurmountable challenge to date. In this work, we construct and synthesize silica-coated Gd2(WO4)3:Yb3+/Ho3+ nanoparticles by one-pot co-precipitation, with uniform distribution (∼130 nm) and enhanced yellow fluorescence. Particularly, the nanoparticles not only possess outstanding temperature sensing performance at biological temperatures in water by utilizing the fluorescence intensity ratio (FIR) method, but also allow a further serviceable contrast effect in vitro and in vivo based on the prominent T1-weighted magnetic resonance (MR) signal of Gd3+. Compared with cisplatin and platinum(iv) (DSP), the Gd2(WO4)3@SiO2 nanoparticles functionalized with DSP (Gd2(WO4)3@SiO2-Pt-PEG) exert higher lethality against CT26 cells and significantly inhibit the growth of tumors at the same concentration of Pt. This effect occurs through the greater level of cell endocytosis. The lethality value of the latter is 10 times higher than the former after the same length of time according to inductively coupled plasma-mass spectrometry (ICP-MS) results. In short, the monodisperse and strongly fluorescent Gd2(WO4)3@SiO2-Pt-PEG nanoparticles are endowed with dual-mode imaging, temperature sensing and anticancer functions, which provide a significant guide for synthesis and bio-application of lanthanide ion-doped oxides.