The quantitative detection of microRNA (miR) and multimode-imaginginduced photothermal therapy in vivo have become the focus of much attention. Platinum (Pt) decorated gold nanorods (AuNR-Pt) and Ag 2 S coresatellite (AuNR-Pt@Ag 2 S) multifunctional nanostructures are fabricated to quantify intracellular miRs (miR-21), near-infrared fluorescence cell quantitative imaging, and tumor ablation in vivo. When combined with miR-21, the nanoassembly displays significant fluorescence intensity in the second window of the near-infrared region (1000-1700 nm) after 808 nm excitation. The Ag 2 S fluorescence intensity has a good linear relationship with the amount of intracellular miR in the range of 0.054-20.45 amol ng RNA −1 and a limit of detection of 0.0082 amol ng RNA −1. The nanoassembly is also used to develop multimodal bioimaging, including near-infrared, X-ray computed tomographic, and photoacoustic imaging in HeLa-tumor-bearing mice. Moreover, the tumors are completely eliminated by the high photothermal capacity of the AuNR-Pt@Ag 2 S assembly. This nanoassembly provides a multifunctional nanoplatform for the ultrasensitive detection of miRs and tumor diagnosis and therapy in vivo.In this context, an AuNR-Pt@Ag 2 S nanoassembly was designed with DNA backbones, [22] and an ultrasensitive and selective miR detection method was developed for living cells. Cell NIR-II fluorescence imaging, X-ray computed tomography (CT) imaging, and photoacoustic (PA) imaging were also used to diagnose the tumors in HeLa-xenograft-bearing mice in vivo. Therefore, the nanoassembly can also be used as a powerful PTT agent, with high photothermal efficiency and safe power doses in the NIR optical window.