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• Gold bipyramids with tunable surface plasmon resonance properties are synthesized. • The morphological yield is over 90% without any purification step. • Gold bipyramids exhibit high absorbance in 740–960 nm. • The functionalized gold bipyramids show great photothermal effect. • Gold bipyramids can be used as for imaging-guided cancer therapy. Monodisperse gold bipyramids (AuBPs) with controlled aspect ratio and tunable surface plasmon resonance (SPR) property have been synthesized using cetyltrimethylammonium bromide (CTAB) and sodium oleate (NaOL). The morphological yield of AuBPs is about 90% without any purification step. The presence of NaOL plays an important role in promoting the morphological yield of AuBPs by pre-reduce Au3+ to Au+. The obtained AuBPs exhibit strong absorbance in the near infrared region (NIR) that can be systematically tuned from 740 nm to 960 nm. After functionalized with polyethylene glycol (PEG), the as-prepared AuBPs have shown excellent photothermal stability and great biocompatibility, which could be used for high contrast computed tomography (CT) imaging and photothermal cancer therapy. This work provides not only a simple method for the synthesis of AuBPs with high morphological yield, but also a promising theranostic agent for cancer therapy. [ABSTRACT FROM AUTHOR]