Akbar, Teuku FawzulJimenez-Rodriguez, Carlos AlejandroBiktimirova, RailiaHermes, IlkaKurth, ThomasPham, My DuyenTsurkan, MikhailFriedrichs, JensMorgan, Francis L. C.Kleemann, HansGuskova, OlgaFreudenberg, UweFratzl, PeterWerner, CarstenTondera, ChristophMinev, Ivan R.2026-03-092026-03-092026-03-09https://opara.zih.tu-dresden.de/handle/123456789/2088https://doi.org/10.25532/OPARA-1107Next generation technologies linking living systems to computers will require materials built on biology, an approach that may address persistent challenges in stable and multimodal information exchange. Here, we present a semi-synthetic hydrogel, designed to emulate key features of native extracellular matrix (ECM) while offering electrically tunable functionality. We engineer interactions between sulfated glycosaminoglycans (sGAGs) and a semiconducting organic polymer (Poly(3,4-ethylenedioxythiophene), PEDOT) within a soft hydrogel network (PEDOT:sGAGh). We demonstrate control over the material’s nanoarchitecture, electrochemical behavior, and biomolecular interactions. In particular, PEDOT:sGAGh exhibits affinity for bioactive proteins, including growth factors, and allows their release or retention to be modulated by low-voltage stimulation. This enables electrical control over macromolecular cues for cell differentiation, a capability not found in natural ECM or conventional conductive hydrogels. These functions are achieved with ultra-low PEDOT content (≈ 1 wt.%), preserving the hydrogel’s tissue-like softness and high water content. The PEDOT:sGAGh material can be integrated as a bioactive coating on electrodes, or into three dimensional organic electrochemical transistors (OECTs). Our results position PEDOT:sGAGh as a versatile platform for realizing biohybrid circuits that bridge molecular signaling and solid-state electronics, thus paving the way for brain-machine interfaces that operate beyond purely electrical modes of interaction.Attribution-NonCommercial-NoDerivatives 4.0 Internationalhttp://creativecommons.org/licenses/by-nc-nd/4.0/4