Photodynamic therapy (PDT) and photothermal therapy (PTT) are two promising methodologies for cancer therapy. Although a variety of materials which can be used in PDT and PTT have been developed in the past decades, those showing the combined effect of PDT and PTT under NIR irradiation are rare. Graphene oxide (GO) and fullerene C₆₀ (denoted as C₆₀ hereafter) with unique physical and chemical properties are promising candidates for PTT and PDT, respectively. Here, by using a stepwise conjugation method, a new GO-C₆₀ hybrid which contains hydrophilic methoxypolyethylene glycol (mPEG) and mono-substituted C₆₀ was constructed for combined PDT and PTT. The hybrid shows good solubility in different environments including physiological solutions. The introduction of C₆₀ to GO did not decrease the photothermal properties of GO, while the conjugation of GO to C₆₀ activated the ability of C₆₀ to generate singlet oxygen (¹O₂) in near infrared (NIR) region in aqueous solution. The GO-C₆₀ hybrid also shows good ability to induce the generation of reactive oxygen species (ROS) in Hela cells. Due to the synergistic effect between GO and C₆₀, GO-C₆₀ hybrid exhibits superior performance in the inhibition of cancer cells compared to both individuals, indicating its high potential in practical applications.