In the recent years, combining advantages of different types of therapy has gained great attention to inhibit tumor growth. For example, codelivery of anti-cancer drug doxorubicin and siRNA by mesoporous silica nanoparticle could overcome drug resistance [1], the efficiency of photodynamic anticancer treatment by photosensitizer hypocrellin was dramatically enhanced because of the photothermal effect by its carrier gold nanocage[2], the combination of doxorubicin and PEGylated grapheme oxide showed a synergistic effect and lower systematic toxicity than doxorubicin alone[3]. In this study, we have developed a new type of molecular-targeted cancer therapy, biological redox enhanced photodynamic therapy (PDT) and photothermal therapy (PTT), which used graphene quantum dots (GQDs) as vehicle to simultaneously deliver anti-cancer drug gadolinium texaphyrin (Gd-TP) and photosensitizer lutetium texaphyrin (Lu-TP) to human lung cancer cells. The presence of paramagnetic Gd(Ⅲ) and the fluorescent from vehicle and drugs could be used to estimate the therapeutic efficiency by MRI and fluorescence imaging. Two water insoluble drugs, Gd-TP and Lu-TP, were loaded onto c(RGDyk) (a targeted peptide) modified orange emission graphene quantum dots via π-conjugative interaction. With the photothermal effect by GQDs and biological redox enhancement by Gd-TP, the PDT efficiency has been increased dramatically, which induced cancer cell death immediately by using very low doses of PDT (Fig. 1). Moreover, with the increased hydrophilicity and solubility of TP in cancer cells, Lu-TP&Gd-TP released from GQDs and exhibit a strong deep-red recovered fluorescence imaging and an enhanced T1 MRI in vivo.After a 765 nm irradiation at a power density of 50 mW/cm2 for 2 min, apoptosis (white arrows) arose when human lung cancer cells were treated with Gd-TP/GQDs-RGD or Lu-TP/GQDs-RGD. Meanwhile, most of the irradiated cells treated with Lu-TP&Gd-TP/GQDs-RGD were necrotic (yellow arrows, Fig. 2). These evidences corroborated the point that the addition of redox active drug Gd-TP strongly promoted apoptosis and/or necrosis in PDT. It has been widely reported that graphene oxide in reduced form could absorb NIR light and produce heat.[4] In this study, one of the graphene derivative, GQDs, were obtained by two steps: carbon nanotubes were oxidized in acid, and then reduced and cut into small pieces of GQDs by microwave-assisted hydrothermal method. In vivo results showed the surface temperature of tumors site on GQDs injected mice arose from 34.6 °C to 39.4°C after irradiation, in contrast to 1.3 °C temperature rise for irradiated tumors on uninjected mice (Fig. 3).The designed probe combined PDT, PTT with biological redox reaction in a new synergistic treatment modalitie, not only fulfills the solubility and selectivity but also constitutes a promising new tumor-targeted theranostics agent that can enhance significantly the efficacy of PDT and real-time dual-modality imaging during targeted therapy.