AbstractTranscranial electrical stimulation is a noninvasive neurostimulation technique with a wide range of therapeutic applications. However, current electrode materials are typically not optimized for this abiotic/biotic interface which requires high charge capacity, operational stability, and conformability. Here, a plant‐based composite electrode material based on the combination of aloe vera (AV) hydrogel and a conducting polymer (CP; poly(3,4‐ethylenedioxythiophene):polystyrene sulfonate, PEDOT:PSS) is reported. This material system is fabricated into films and provides biocompatibility, conformability, and stability, while offering desirable electrical properties of the PEDOT:PSS. AVCP films are also molded onto the rough surface of the skull leading to a mechanically stable and robust interface. The in vivo efficacy of the AVCP films is verified to function as stimulating and recording electrodes by placing them on the skull of a rat and concomitantly inducing focal seizures and acquiring the evoked neural activity. AVCP films pave the way for high‐quality biological interfaces that are broadly applicable and can facilitate advances in closed‐loop responsive stimulation devices.