Nanoprobes are rapidly becoming potentially transformative tools on disease diagnostics for a wide range of in vivo computed tomography (CT) imaging. Compared with conventional molecular-scale contrast agents, nanoparticles (NPs) promise improved abilities for in vivo detection. In this study, novel polyethylene glycol (PEG)-functionalized Au nanoparticles with star shape (AuNS@PEG) with strong X-ray mass absorption coefficient were synthesized as CT imaging contrast agents. Experimental results revealed that AuNS@PEG nanoparticles are well constructed with ultrasmall sizes, effective metabolisability, high computed tomography value, and outstanding biocompatibility. In vivo imaging also showed that the obtained AuNS@PEG nanoparticles can be efficiently used in CT-enhanced imaging. Therefore, the synthesized contrast agent AuNS@PEG nanoparticles as a great potential candidate can be widely used for CT imaging.