Multifunctional theranostic platforms, especially single component-based platforms, enable both cancer treatment and real-time imaging as well as enhance the efficiency of treatment. In this study, 50 nm Mo2C nanospheres were explored as a "one-for-all" theranostic agent. The light-harvesting of Mo2C covered the entire near infrared region, and NIR irradiation concurrently triggered hyperthermia and reactive oxygen species (ROS) production; thus, synergistic outcomes of photothermal and photodynamic therapy could be realized. Both in vitro and in vivo experiments have confirmed the superiority of the synergistic phototherapy in killing cancer cells and removing solid tumors; moreover, Mo2C proposed herein has been proven to be applicable as a photoacoustic imaging and CT imaging contrast agent for in vivo tumor depiction; furthermore, Mo2C demonstrates excellent biocompatibility, showing minimal hematotoxicity and tissue toxicity. A theoretical simulation performed by density functional theory revealed that the metallic character and the interband/intraband transition of Mo2C accounted for its broad photoabsorption. The antitumor mechanism of Mo2C was investigated on a solid tumor by B-mode ultrasonography (US) and magnetic resonance imaging (MRI), revealing a typical liquefactive necrosis process; hence, herein, the dual-imaging guided phototherapy was efficiently mediated by Mo2C.