We herein report aqueous fabrication of well-defined Au@Cu2-xE (E = S, Se) core@shell dual plasmonic supraparticles (SPs) for multimodal imaging and tumor therapy at the in vivo level. By means of a modified self-limiting self-assembly based strategy, monodisperse core@shell dual plasmonic SPs, including spherical Au@Cu2-xS SPs, Au@Cu2-xSe SPs, and rod-like Au@Cu2-xS SPs, are reliably and eco-friendly fabricated in aqueous solution. Due to plasmonic coupling from the core and shell materials, the as-prepared hybrid products possess an extremely large extinction coefficient (9.32 L g-1 cm-1 for spherical Au@Cu2-xS SPs) at 808 nm, which endows their excellent photothermal effect. Furthermore, the hybrid core@shell SPs possess the properties of good biocompatibility, low nonspecific interactions, and high photothermal stability. So, they show favorable performances for photoacoustic imaging and X-ray computed tomography imaging as well as photothermal therapy of tumors, indicating their application potentials in biological field.