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Enzymatic biofuel cells (EBFCs) are attractive power sources capable of utilizing biomolecules to generate electrical power. However, their practical utility is limited because of their relatively low power output and short lifetime, which arise from the low enzyme loading capacity on the support materials, activity loss during enzyme immobilization, intrinsically poor enzyme stability, and limited substrate and electron transport. Nanobiocatalytic approaches, in which enzymes are incorporated with nanostructured supports, have been recognized as a potent solution to resolve these limitations. They construct high-performance enzyme electrodes utilizing the affirmative characteristics of the materials coupled with appropriate immobilization strategies. In this review, the roles of nanostructured supports and catalytic mechanisms for generating biofuel-driven electrical power, the recent research progress on EBFCs based on widely investigated nanocarbons, nanoparticles, and polymeric nanofibers, and newly emerged metal–organic frameworks, nanoflowers, and other nanohybrids are discussed. The current challenges and prospects for utilizing nanostructured supports in EBFCs are also discussed.