Second near-infrared (NIR-II) fluorescence imaging is a recently emerged technique and is highly useful for accurate diagnosis of cancer. Although a diverse array of fluorescent nanomaterials have been developed to enable NIR-II fluorescence in various situations, they normally fail to unify the clinical techniques, such as computed tomography (CT) and magnetic resonance imaging (MRI). Therefore, exploiting multimodal agents to integrate the newly emerged NIR-II fluorescence and traditional clinical techniques would be of key significance. Here, we report a rational fabrication of neodymium (Nd)-doped gadolinium tungstate nanoparticles (NPs) that are subsequentially decorated with a hydrophilic layer and demonstrate that they can achieve the harmonious integration of NIR-II fluorescence imaging, CT, and MRI. The NIR-II fluorescence emission was activated by an incident light with discrete wavelength ranging from 250 to 810 nm. NIR-II fluorescence-CT-MRI associated trimodal imaging was subsequently demonstrated for breast cancer by an 808 nm laser, along with the estimation of NIR-II fluorescence imaging for cervical cancer. The integration of newly emerged and traditional clinical imaging techniques highlights the huge potential of rare-earth-doped NPs for multimodal imaging of different types of cancer.