The development of the advanced imaging probe holds the key to the achievement of target imaging and metastasis tracing. The bismuth based nanoprobe has been regarded as the most promising X-ray computed tomography probe due to its largest X-ray attenuation coefficient. Accordingly, the bismuth nanoparticles with controllable size distribution and light weight have been fabricated through a one pot synthesis strategy. The surface modification can be easily conducted with the polyethylene glycol to make the nanoparticles hydrosoluble and biocompatible. More importantly, the Bi nanoparticles can be excited by light to conduct excitation wavelength dependent emission in the visible (Vis) and near-infrared (NIR) region, which makes it possible to utilize it for fluorescence imaging. Under the detection of the multimode CT/fluorescence imaging, the long circulation time of the Bi nanoparticles and its specific accumulation at the liver and intestine can be visually displayed. The facile and large scale preparation method, unique luminescence property, and multimode imaging function endow the Bi nanoparticles with promising applications in clinical diagnosis. ©