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ARTICLE This journal isThe GNS-V2O5/TiO2 composite, as a new class of nanoarchitecture, have been successfully fabricated by a facile hydrothermal process followed by a sol-gel technique. Such nanoarchitecture is made up of V2O5/TiO2 core/shell nanorods, chemically anchored on graphene nanosheets (GNS). High-resolution scanning transmission electron microscopy shows that these core/shell nanoparticles consist of core V2O5 nanorods of diameter 120 nm to 140 nm, covered by TiO2 shell of about 15 nm to 20 nm thickness. Large quantities of core/shell nanostructure materials are uniformly embedded on the surface of GNS. These new nanoarchitectures consists of two different kinds of metal oxides, that is V2O5 and TiO2 which are electrostatically coupled with each other and decorated on the GNS by chemical bonding between C-Ti confirmed by Zeta potential analyzer and XPS studies, respectively. The sunlight-active photocatalytic properties of the GNS-V2O5/TiO2 nanoarchitectures have been evaluated by photodegradation of acridine orange (AO) dye in an aqueous medium. Results show that the enhancement in the photocatalytic activity was attributed to the synergetic effect and also the chemical bonding leads to the interfacial charge transfer effect between GNS-semiconductor interfaces. It remarkably increases the spatial condition for charge transport and also increases the number of holes participating in the photodegradation process. This new nanoarchitecture exhibits an efficient photocatalytic activity and very high stability, holding great potential as a highly stable and reusable material for energy, water splitting, and environmental cleaning applications. nm corresponds to (101) plane of anatase TiO 2 . 14,28 It demonstrates that the exposed facets of TiO 2 were embedded onto the surface of graphene indicating that there was an interaction between Ti atoms with GNS. Journal Name ARTICLEThis journal is