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Abstract: Indocyanine green (ICG) is an effective light absorber for laser‐mediated photodynamic therapy. However, applications of ICG are limited due to its rapid degradation and poor photostability in water. Herein, we report the development of a multifunctional nanoplatform by coating ICG on the surface of single‐walled carbon nanohorns (SWNHs) through π–π stacking, obtaining SWNH‐ICGs with high solubility and stability under physiological conditions. The SWNH‐ICGs could be used as a single nanoplatform to simultaneously produce satisfactory hyperthermia and reactive oxygen species under near‐infrared (NIR) laser irradiation. In addition, the SWNH‐ICGs not only improved the photostability of ICG in different media, but also protected it from light degradation. The SWNH‐ICGs exhibited highly efficient thermal/photoacoustic (PA) imaging‐guided photothermal therapy (PTT) and photodynamic therapy (PDT) effects, even under low‐power laser irradiation (0.3 W cm−2) in vitro. Combined PTT and PDT effectively killed triple‐negative breast cancer 4T1 cells, demonstrating a markedly improved and synergistic therapeutic effect compared to PTT or PDT alone. Furthermore, significant tumor growth inhibition as well as tumor cell death were observed following PTT/PDT at 808 nm laser irradiation, confirming the synergistic effects of SWNH‐ICGs over free ICG in vivo. This facile and simple methodology for thermal/PA imaging‐guided PTT/PDT suggests that SWNH‐ICGs may serve as an effective nanoplatform for cancer therapy. [ABSTRACT FROM AUTHOR]