Multimodal neural interfaces include combined functions of electrical neuromodulation and synchronic monitoring of neurochemical and physiological signals in one device. The remarkable biocompatibility and electrochemical performance of polystyrene sulfonate-doped poly(3,4-ethylenedioxythiophene) (PEDOT:PSS) have made it the most recommended conductive polymer neural electrode material. However, PEDOT:PSS formed by electrochemical deposition, called PEDOT/PSS, often need multiple doping to improve structural instability in moisture, resolve the difficulties of functionalization, and overcome the poor cellular affinity. In this work, inspired by the catechol-derived adhesion and semiconductive properties of polydopamine melanin (PDAM), we used electrochemical oxidation polymerization to develop PDAM-doped PEDOT (PEDOT/PDAM) as a bioactive multimodal neural interface that permits robust electrochemical performance, structural stability, analyte-trapping capacity, and neural stem cell affinity. The use of potentiodynamic scans resolved the problem of copolymerizing 3,4-ethylenedioxythiophene (EDOT) and dopamine (DA), enabling the formation of PEDOT/PDAM self-assembled nanodomains with an ideal doping state associated with remarkable current storage and charge transfer capacity. Owing to the richness of hydrogen bond donors/acceptors provided by the hydroxyl groups of PDAM, PEDOT/PDAM presented better electrochemical and mechanical stability than PEDOT/PSS. It has also enabled high sensitivity and selectivity in the electrochemical detection of DA. Different from PEDOT/PSS, which inhibited the survival of human induced pluripotent stem cell-derived neural progenitor cells, PEDOT/PDAM maintained cell proliferation and even promoted cell differentiation into neuronal networks. Finally, PEDOT/PDAM was modified on a commercialized microelectrode array system, which resulted in the reduction of impedance by more than one order of magnitude; this significantly improved the resolution and reduced the noise of neuronal signal recording. With these advantages, PEDOT/PDAM is anticipated to be an efficient bioactive multimodal neural electrode material with potential application to brain-machine interfaces.