Branched anisotropic gold nanostructures present distinguished performance acting both as contrast agents for photoacoustic imaging and as active agents for photothermal therapies. Despite advances in their fabrication methods, the synthesis of such gold nanomaterials in a simple and reproducible way is still a challenge. In this paper, we report the development of branched anisotropic gold nanoparticles, the so-called gold nanoflowers (AuNFs), as near-infrared active theragnostic materials for cancer therapy and diagnosis. In situ chemical synthesis of the AuNFs was optimized to obtain monodisperse nanoflowers with controllable size and optical properties. Upon varying the temperature and gold ion concentrations, it was possible to tune the optical activity of the nanoparticles from 590 to 960 nm. The AuNFs exhibited good stability in the cell culture medium, and under laser irradiation. Photoacoustic imaging revealed that the NFs could be imaged in phantom systems even at low concentrations. In vitro tests revealed that the nanoflowers were effective in the photothermal therapy of a rat hepatocarcinoma (HTC) cell lineage. In addition, no toxicity was observed to mouse fibroblast (FC3H) cells incubated with the AuNFs. Our results reveal a simple method to synthesize branched anisotropic gold nanostructures, which is a promising platform for photothermal and photoacoustic therapies.