4386www.MaterialsViews.com wileyonlinelibrary.com strategy for the successful cancer treatment. [ 2 ] On the one hand, stimuli-responsive drug delivery systems (DDSs) can realize the on-demand drug release triggered by inner physiological changes (pH, redox, enzyme, competitive binding, etc.) and/or external irradiations (light, magnetic, electronic fi eld, ultrasound, etc.), thus the side-effects caused by toxic drugs to normal tissues can be effectively mitigated and the therapeutic effi cacy against cancer cells can be signifi cantly enhanced. [ 3 ] On the other hand, stimuli-enhanced diagnostic imaging, such as magnetic resonance imaging (MRI), ultrasonography, fl uorescence, and so on, can effectively improve the imaging performances of contrast agents (CAs) for accurate tumor imaging and detection. [ 4 ] However, the construction of multifunctional nanosystems with concurrent multiple stimuli-responsive drug release and diagnostic imaging still remains a great technical challenge though it is of substantial signifi cance for realizing the simultaneous diagnostic imaging and therapy (designated as theranostic) for successful cancer treatments. Exfoliated graphene oxide (GO) nanosheets, a parent material of graphene with unique free-standing two-dimensional crystallized structure and one-atom thickness, has been extensively explored in drug delivery, [ 5 ] gene transportation, [ 6 ] molecular imaging, [ 7 ] biosensing [ 8 ] and photothermal/photodynamic therapy, [ 9 ] mainly due to its high biocompatibility and unique physical/chemical properties such as excellent aqueous processability, abundant surface chemistry, near-infrared light
Construction of multifunctional stimuli-responsive nanosystems intelligently responsive to inner physiological and/or external irradiations based on nanobiotechnology can enable the on-demand drug release and improved diagnostic imaging to mitigate the side-effects of anticancer drugs and enhance the diagnostic/therapeutic outcome simultaneously. Here, a triple-functional stimuli-responsive nanosystem based on the co-integration of superparamagnetic Fe 3 O 4 and paramagnetic MnO x nanoparticles (NPs) onto exfoliated graphene oxide (GO) nanosheets by a novel and effi cient double redox strategy (DRS) is reported. Aromatic anticancer drug molecules can interactwith GO nanosheets through supramolecular π stacking to achieve high drug loading capacity and pH-responsive drug releasing performance. The integrated MnO x NPs can disintegrate in mild acidic and reduction environment to realize the highly effi cient pH-responsive and reduction-triggered T 1weighted magnetic resonance imaging (MRI). Superparamagnetic Fe 3 O 4 NPs can not only function as the T 2 -weighted contrast agents for MRI, but also response to the external magnetic fi eld for magnetic hyperthermia against cancer. Importantly, the constructed biocompatible GO-based nanoplatform can inhibit the metastasis of cancer cells by downregulating the expression of metastasis-related proteins, and anticancer drug-loa...