Bilayered PEDOT:PSS–Collagen Scaffolds as Functional Architectures for Tissue Engineering

ABSTRACT Biomaterial‐based scaffolds that combine cell‐supportive microenvironments with complementary functional properties are important for advancing tissue‐engineering platforms. Here, we report a bilayered scaffold that integrates a reconstituted fibrillar collagen matrix with a conductive polymer, poly(3,4‐ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS), combining a biomimetic extracellular matrix with an electrically conductive 3D architecture. The bilayer design maintains the characteristic organization and structural integrity of each phase, preserving the collagen fibrillar network, while the PEDOT:PSS compartment provides a conductive compartment compatible with electrochemical measurements. Varying collagen concentration enables tailoring of the fibrillar density and pore architecture of the collagen compartment, with corresponding effects on swelling, mechanical behavior, and electrochemical response. As a proof of concept, in situ electrochemical impedance measurements are used to follow time‐dependent changes during fibroblast–epithelial co‐culture. Measured impedance progression is consistent with epithelial organization and tight‐junction formation, as visualized by immunofluorescence imaging. This proposed bilayered scaffold provides a versatile materials strategy for integrating 3D biomimetic and conductive architectures while preserving their individual characteristics, offering opportunities for advanced 3D in vitro tissue models and organotypic interfaces.