Nanoscale components at neural interface are crucial factors for neural devices due to the complex nanoscale structure of neural tissue. Nitrogen-doped graphene (g-C3N4) was prepared and applied as a candidate material for the surface modification of neural electrodes. To better explore the practical applications of g-C3N4, a conducting polymer of poly(3,4-ethylenedioxythiophene) (PEDOT) was employed and a nanoporous composite of g-C3N4/PEDOT was achieved with excellent electrochemical performance including low interfacial impedance, high electric capacity, and long-term stability. Investigation revealed that the enhanced performance of the composite was attributed to its unique nanostructure, which was confirmed by field emission scanning electron microscopy, as well as the synergistic effect of the two components. Moreover, in vitro experiments demonstrated that g-C3N4/PEDOT promoted robust cell growth, possessing excellent biocompatibility. Our study validates that the g-C3N4/PEDOT nanocomposite is a promising candidate material to construct the interface between neural tissue and neural electrodes. POLYM. ENG. SCI., 58:1548-1554, 2018. (c) 2017 Society of Plastics Engineers