The ability to sense and stimulate cellular and tissue electrophysiology is fundamental to input/output bioelectronics. Their functionality is primarily governed by the structural and functional properties of the constituent electrode materials. Conventional electrode materials are hindered by their twodimensional topology, high electrochemical impedances, low charge injection capacities, and limited stability over chronic timescales. Here, we propose a strategy for obtaining high-surfacearea hybrid-nanomaterial for efficient I/O bioelectronics by conformally templating conductive polymer poly(3,4-ethylenedioxythiophene)−polystyrene sulfonate (PEDOT:PSS) onto nanowiretemplated three-dimensional (3D) fuzzy graphene (NT-3DFG). The result is a high-performance electrode material that can leverage the exceptional surface area of NT-3DFG and the volumetric charge storage properties of PEDOT:PSS. Owing to its high surface area, NT-3DFG microelectrodes exhibit lower electrode impedance and up to 35-fold greater charge injection capacity (CIC) compared to conventional metal microelectrodes. Conformally templating PEDOT:PSS onto NT-3DFG further reduces electrode impedance and enhances CIC by 125-fold compared to conventional metal microelectrodes. Moreover, the NT-3DFG-based nanomaterials exhibit high functional stability. Our results highlight the importance of extrapolating electrode topography to 3D and developing hybrid nanomaterials for miniaturized microelectrodes for functional bioelectronics.