A bottom‐up approach is taken to confer multidimensional structure to conductive polymers by attaching thiophene monomers to peptides predicted to self‐assemble into a biomimetic, fibrous nanostructure. A library of 12 peptides containing covalently attached thiophene monomers are synthesized. Peptide sequences capable of robust self‐assembly and hydrogel formation in aqueous media are further polymerized in situ and the physical and electrical properties are characterized. The resulting hybrid materials have conductivities in the range of 10−2 to 10−3 S cm−1 and possess moduli in the range of several tissue types, making them potential candidates for use in tissue engineering and bioelectronic applications.