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The reconstitution of an apo-flavoenzyme, apo–glucose oxidase, on a 1.4-nanometer gold nanocrystal functionalized with the cofactor flavin adenine dinucleotide and integrated into a conductive film yields a bioelectrocatalytic system with exceptional electrical contact with the electrode support. The electron transfer turnover rate of the reconstituted bioelectrocatalyst is ∼5000 per second, compared with the rate at which molecular oxygen, the natural cosubstrate of the enzyme, accepts electrons (∼700 per second). The gold nanoparticle acts as an electron relay or “electrical nanoplug” for the alignment of the enzyme on the conductive support and for the electrical wiring of its redox-active center.