Nanoparticles of noble metals dispersed on solid support have been extensively utilized for catalyzing chemical reactions for energy conversion, environmental remediation, and chemical industry for their remarkable catalytic performance. [1][2][3][4] To maneuver the catalytic performance of these materials, tremendous efforts have been focused on the control of metal nanoparticles, including size and shape, [5][6][7] composition, [8] and chemical ordering. [9] At the meantime, the influence of the support on catalytic properties maximizing the number of active sites accessible for reaction have been well recognized. For example, the size distribution [10] and structural stability [11] of metal nanoparticles could be adjusted via the selection of the support. Furthermore, encapsulation of the metals by support species under high temperature treatment are widely observed, which finally results in the establishment of the classical strong metal-support interaction (SMSI). [12] However, the physicochemical interaction between metal and support cannotThe catalytic properties of nanometals are strongly dependent on their electronic states which, are influenced by the interaction with the supports. However, a precise manipulation of the electronic interaction is lacking, and the nature of the interaction is still ambiguous. Herein, using Au/ZnFe x Co 2−x O 4 (x = 0-2) as a model system with continuously tuned Fermi levels of supports, the electronic structure of the Au catalyst can be precisely controlled by changing the Fermi level of the support, which arises from the charge redistribution between the two phases. A higher Fermi level of ZnFe 2 O 4 support makes nano-Au negatively charged and thus facilitates the oxidation of CO, and in contrast, a lower Fermi level of ZnCo 2 O 4 support makes nano-Au positively charged and is preferential to the oxidation of benzyl alcohol. This work represents a solid step towards exploration of advanced catalysts with deliberate design of electronic structure and catalytic properties.