Indocyanine green-loaded mesoporous silica-coated gold nanorods (ICG-loaded Au@SiO2) were prepared for the dual capability of X-ray computed tomography (CT) and fluorescence imaging. X-ray CT scanning showed that ICG-loaded Au@SiO2 could provide significant contrast enhancement; Near-infrared fluorescence generated by the nanomaterial was present up to 12 h post intratumoral injection, thus enabling ICG-loaded Au@SiO2 to be used as a promising dual mode imaging contrast agent. Multiplexed images can be more easily obtained with this novel type of multimodal nanostructure compared with traditional contrast agents. The dual mode imaging probe has great potential for use in applications such as cancer targeting, molecular imaging in combination with radiotherapy, and photothermolysis.