An engineered metallic nanostructure is an excellent candidate for "theranosis" of cancer, having intrinsic properties of multimodal imaging and therapy. Toward this target, the development of silver-neodymium bimetallic nanoparticles (Ag-Nd BNPs) via microwave-assisted polyol synthesis is presented. The resultant Ag-Nd BNPs exhibit good monodispersity with average size of 10 nm, fluorescence in the near-infrared (NIR) region, and magnetic properties. The Ag-Nd BNPs also validate MRI, CT, and NIR trimodal imaging ability and enunciate valuable temperature response upon irradiation under a NIR laser. Aided by chitosan functionalization on the surface, the Ag-Nd BNPs deliver good biocompatibility and also promote the loading of paclitaxel, an anticancer drug. Isothermal titration calorimetry affirms the combination of strong binding affinity of drug and high loading efficiency of 7 drug molecules per nanoparticle. Moreover, Ag-Nd BNPs also illustrate a highly efficient photothermal effect in PBS. Therefore, the synergistic effects of paclitaxel and the photothermal effect make BNPs excellent "combined therapeutic agents", and also give them the important ability to destroy cancer cells in vitro at very low dose in comparison to single therapy. Thus, the Ag-Nd BNPs unveil a combination of MRI/CT/NIR imaging and chemo-photothermal therapy that ensures accurate diagnosis at an early stage and comprehensive eradication of tumor cells without affecting healthy cells.