The localized surface plasmon resonance (LSPR) of plasmonic nanomaterials is highly dependent on their structures. Going beyond simple shape and size, further structural diversification demands the growth of non-wetting domains. Now, two new dimensions of synthetic controls in Au-on-Au homometallic nanohybrids are presented: the number of the Au islands and the emerging shapes. By controlling the interfacial energy and growth kinetics, a series of Au-on-AuNR hybrid structures are successfully obtained, with the newly grown Au domains being sphere and branched wire (nanocoral). The structural variety allowed the LSPR to be fine-tuned in full spectrum range, making them excellent candidates for plasmonic applications. The nanocorals exhibit black-body absorption and outstanding photothermal conversion capability in NIR-II window. In vitro and in vivo experiments verified them as excellent photothermal therapy and photoacoustic imaging agents.