In this paper, we reported Au@Cu2S nanocrystals in the aqueous phase with a core/shell structure and dBSA encapsulation. The dBSA-Au@Cu2S crystals formed with an average size of approximately 9 nm. There was a strong absorption in the near-infrared (NIR) field located at 1348 nm, and they exhibited low toxicity in the in vitro tests. Furthermore, we demonstrated that dBSA-Au@Cu2S could be used for optical coherence tomography (OCT). The in vivo experimental results show that the OCT signal increased as the concentration of nanocrystals increased. In this research, we revealed that these core/shell-structured nanocrystals along with their low toxicity and excellent biocompatibility could be a valuable tool for current and future contrast-enhanced in vivo studies.